- Email: [email protected]
Review of pre-combustion capture and ionic liquid in carbon capture and storage
Applied Energy 183 (2016) 1633–1663
Contents lists available at ScienceDirect
Applied Energy journal homepage: www.elsevier.com/locate/apenergy
Review of pre-combustion capture and ionic liquid in carbon capture and storage Wai Lip Theo a, Jeng Shiun Lim a,b,⇑, Haslenda Hashim a,b, Azizul Azri Mustaffa a,b, Wai Shin Ho a,b a b
Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia Process Systems Engineering Centre (PROSPECT), Research Institute for Sustainable Environment, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia
h i g h l i g h t s Important carbon capture technologies for pre-combustion capture. Review of physical solvents for pre-combustion capture with physical absorption. Review of solubility models for carbon capture. Challenges and future prospect of pre-combustion capture. Research gaps in ionic liquid-based UNIFAC model development.
a r t i c l e
i n f o
Article history: Received 20 July 2016 Received in revised form 5 September 2016 Accepted 26 September 2016
Keywords: Carbon capture and storage (CCS) Pre-combustion capture Ionic liquid (IL) UNIFAC model Computer-aided molecular design (CAMD) Review
a b s t r a c t Global warming issue, which increasingly aggravates over time, necessitates the carbon capture and storage (CCS) technology for its efficient mitigation. Among the major CCS technologies, post-combustion capture is the most established and commonly employed. However, it poses several energy and environment-related problems. As such, research and development of the pre-combustion carbon capture has been conducted to overcome the drawbacks of this conventional approach, and incorporation of ionic liquid (IL) has been increasingly given attention. This paper intends to review the carbon dioxide separation technologies and those related to IL in pre-combustion capture, pre-combustion capture research progress, pilot plant and commercial facilities, as well as modelling approach with special focus on the computer-aided molecular design (CAMD). In the last aspect, emphasis is given to the IL-based UNIFAC model, and key research gaps are identified from the review as general guidelines for the future research work and development in this particular field. Ó 2016 Elsevier Ltd. All rights reserved.
Contents 1. 2. 3.
4.
5.
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Introduction to pre-combustion carbon capture technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Important global research progress, pilot plants and commercial facilities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1. Pre-combustion capture research progress . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2. Pilot plant overview . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3. Commercial scale plant overview. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Carbon dioxide separation technologies for pre-combustion carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.1. Physical absorption technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.2. Adsorption technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.3. Membrane technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.4. Cryogenic separation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.5. Comparison of CO2 separation technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Ionic liquid in carbon capture and storage (CCS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
⇑ Corresponding author at: Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia. E-mail address: [email protected] (J.S. Lim). http://dx.doi.org/10.1016/j.apenergy.2016.09.103 0306-2619/Ó 2016 Elsevier Ltd. All rights reserved.
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6.
Solvent design optimisation for pre-combustion carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6.1. Review of solubility models for carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6.2. Review of ionic liquid (IL)-based UNIFAC model. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7. Summary of research gaps. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8. Challenges of pre-combustion carbon capture technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.1. Commercial viability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.2. Financial constraint . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.3. Governance and regulatory framework . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.4. Technological constraint . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9. Future prospect of pre-combustion carbon capture. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
1. Introduction Global warming has become more pronounced due to the immense carbon emissions from the fossil fuel-centred energy supply-demand chain worldwide. Currently, significant energy demand has continuously increased with increasing economic affluence of the modern society. According to International Energy Agency (IEA) [1], overall global primary energy demand in 2011 was already in the order of 550 exajoules. Moreover, it was anticipated to increase by 36% from 2008 to 2035 [2]. As a result, the global consumptions of petroleum, coal and natural gas were expected to increase at the annual rates of 1.2%, 1.4%, and 2.0% to reach the projected demands of 114 million barrels per day, 7000 million tonnes of coal equivalence, and 5000 billion cubic meters by 2035 [3]. This trend had led to carbon emissions up to 33.4 billion tonnes in 2011 [4]. According to Intergovernmental Panel on Climate Change (IPCC) [5], the global carbon dioxide concentration, without mitigation approach in place, would reach the range of 600–1550 ppm in 2030. Such transition in the atmospheric concentration of carbon dioxide has unequivocally led to warming of global climate system, leading to an increment in the global average temperature by 0.8 °C since 1880 [6]. If the problem were to be left to aggravate itself, the global mean surface temperature might increase by 2.5–7.8 °C by 2100, with consideration of climate uncertainties [7]. The global warming phenomenon would in turn exert negative impacts on the physical environment (i.e. increased global average temperature, sea level elevation, coastal region erosion [5], water cycle disruption, abnormal climate pattern, and ocean acidification [8]), biological ecosystem (i.e. endangerment of climate-sensitive and arctic species, wildfire destruction of fauna species, and occurrence of oceanic dead zones [8]), and human welfare (i.e. reduced water availability [9], food crisis [10], prevalence of water-borne diseases [11], and increased mortality associated with extreme weathers [5]). These crises, if left unresolved, could endanger the natural ecosystem and human civilisation. For effectively mitigating the global warming impacts, IPCC [7] indicated the need of keeping the global mean temperature elevation below 2 °C relative to the pre-industrial level. This would necessitate GHG emissions reduction by 40–70% as compared to 2010 level by 2050, and subsequently by 100% in 2100 [7]. Increased commitment has been seen through intensification of GHG emissions mitigation plans and strategies since 2012, whereby 67% reduction target of the global GHG emissions was officially enforced via regulations and policies [7]. The common policy instruments for GHG emissions reduction, especially for industrial and energy sectors, include voluntary approaches (VA), emissions trading, and emissions taxes [12]. Various adaptation and mitigation plans were recommended and evaluated by IPCC [7], and they encompass the following:
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i. Employment of low carbon intensive energy resources in place of coal, i.e. nuclear [13], natural gas [14], hydrogen fuel cell [15], and renewable energy resources (i.e. solar, wind, hydro, tidal, biomass and geothermal energy) [16]. ii. Enhancing energy efficiency of urban, industrial, and transportation sectors [17], and promoting energy conservation. iii. Geoengineering approaches, inclusive of carbon dioxide removal (CDR) and solar radiation management [18]. While there have been intensive researches devoted to exploring cleaner fuels and more efficient power generation technologies, the solutions however are still too expensive to be commercialised and widely applied. With more than 80% of overall energy demand currently being fulfilled by fossil fuel-based power plants, largescale emissions of carbon dioxide would be inevitable despite having these technological breakthroughs. Therefore, carbon sequestration via carbon capture and storage (CCS) approach is still the predominant strategy for global warming mitigation since it is technically and economically feasible with current cost range of USD 200–250 per tonne of carbon [19], has high carbon dioxide capture efficiency of more than 80%, and is compatible for intensive carbon dioxide point emission sources (i.e. power plants and heavy manufacturing industries) [20]. CCS is a large-scale separation of carbon dioxide from its significant sources followed by long-term isolation from the atmosphere and probably appropriate utilisation. It is an end-of-pipe solution tailor-made for the scenario whereby substantial emissions of carbon dioxide, associated with ever increasing global energy demand, industrial intensification and reliance on fossil fuel, are inevitable [21]. This approach is typically compatible for carbon sequestration from large-scale carbon dioxide point sources. The potential sectors for incorporation of CCS include power generation and heavy chemical manufacturing sectors.
Fig. 1. Global energy-related anthropogenic carbon dioxide emissions from 1990 to 2040 [22].
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As illustrated in Fig. 2, the energy-related anthropogenic carbon dioxide emissions had reached 32.27 billion tonnes by 2012. This figure is anticipated to elevate to 35.63 billion tonnes by 2020 and 43.22 billion tonne by 2040, whereby the majority of projected increase in carbon dioxide emissions is contributed by developing countries excluded from the Organisation for Economic Cooperation and Development (OECD) (as illustrated in Fig. 1) [22]. With all planned commercial CCS facilities worldwide, only 33.4 million tonnes of annual carbon capture capacity could be achieved by 2020, which is equivalent to 0.09% of the total estimated carbon emissions. For practical stabilisation of greenhouse effect, expansion of CCS technology would be in dire need.
In general, CCS technology could be categorised into postcombustion, pre-combustion and oxyfuel combustion capture types, as compared in Table 1. Fig. 2 illustrates the statistics of constructed commercial carbon capture facilities and capture capacity worldwide, and the details of the statistics shown are presented in Tables 2 and 3. It shall be noted that there is currently no operational full-scale CCS plant applying the oxyfuel combustion capture system. To date, post-combustion capture has been the most established CCS strategy with proven pilot projects and commercial scale plants. Solvent development and process intensification for post-combustion carbon capture using chemical absorption are
Table 1 Comparison of carbon capture technologies [23]. Aspect
Post-combustion capture
Pre-combustion capture
Oxyfuel combustion capture
Technology maturity level
Highly mature with numerous established applications at full-scale commercial plants
Well-established in process industries (typically water-gas shift reaction coupled with acid gas removal (AGR) process); Establishment of full-scale CCS plants under progress (mostly still in construction phase)
No full-scale oxyfuel-based CCS plants in operation; Limited to pilot-scale operations to date
Technical advantages
Highly compatible for retrofitting of existing power plants (enabling the continued use of common power generation technology i.e. pulverised coal); Comprehensive research in place to improve energy efficiency of postcombustion carbon capture equipment
Less energy-intensive carbon dioxide separation process (due to lower gas volume, higher pressure, and higher carbon dioxide concentration); More technologies commercially available for AGR process; Lower water consumption (as compared with post-combustion capture); Generation of hydrogen/synthesis gas as alternative fuel
Minimal emission of pollutants; No requirement of on-site chemical operations; Robust i.e. compatibility with a wide variety of coal fuels; Easier and simpler retrofit compared to post-combustion capture system; High carbon capture efficiency (on cost per tonne carbon dioxide sequestered basis) due to high carbon dioxide concentration; Reduced equipment size requirement; High maturity of air separation technology; High compatibility with conventional, high-efficient steam cycle without significant modifications; Highly established auxiliary equipment i.e. rotating equipment and heat exchanger
Technical disadvantages
Separation constraint imposed by low carbon dioxide partial pressure in flue gas; Commercially available amine scrubbing technology is often of small-scale and requires substantial upscaling; Significant energy penalty of amine scrubbing process (i.e. loss of 30% overall power output); Requirement of energy-intensive carbon dioxide compression; Most sorbent technologies are less robust with high performance requirement; Extensive water consumption
Significant energy loss due to sorbent regeneration (yet lower than that of post-combustion capture); Limited commercial availability of Integrated Gasification Combined Cycle (IGCC) technology; High auxiliary system requirement by IGCC technology; Syngas temperature swingassociated heat transfer problem; Reduced efficiency associated with hydrogen-fuelled gas turbine application
Infeasible development of sub-scale oxyfuel combustion capture technology; Net power output reduction due to energy-intensive air separation unit (ASU) and carbon dioxide compression; Technical uncertainties associated with operation of full-scale plant remain unresolved; Requirement of air-tight installation to avoid air leakage (or carbon dioxide leakage due to overpressurised operation); Possible corrosion problem
Economic aspect
High capital and operational expenditures due to large equipment size requirement (i.e. large flue gas volume)
IGCC capital cost is far higher than that of conventional coal power plant; High capital and operational expenditures for sorbent technology
High capital cost for air separation technology
Gas-fired: USD 1180 per kW Coal-fired: USD 1820 per kW
Gas-fired: USD 1530 per kW Coal-fired: USD 2210 per kW
Gas-fired: USD 0.097 per kW Coal-fired: USD 0.069 per kW
Gas-fired: USD 0.100 per kW Coal-fired: USD 0.078 per kW
Capital costa Gas-fired: USD 870 per kW Coal-fired: USD 1980 per kW Electricity costa Gas-fired: USD 0.080 per kW Coal-fired: USD 0.075 per kW a
Source: International Energy Agency Greenhouse Gas Programme [24].
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Fig. 2. Statistics of commercial carbon capture facilities worldwide.
well developed [42], and various solid sorbent technologies are continuously researched for its improvement [43]. However, it suffers several drawbacks, i.e. high regeneration enthalpy, thermal and oxidative degradation of amine-based solvents, and low carbon dioxide partial pressure constraint. Pre-combustion capture seems to be a promising alternative for overcoming these predicaments. As compared to extensive review by Thambimuthu et al. [44] and Kumar et al. [45], this review shall provide additional information about the current research programmes and advances in pre-combustion carbon capture development, pilot plant and commercial facility development status. Moreover, for modelling development of pre-combustion carbon capture optimisation, solubility model and particularly ionic liquid (IL)-based UNIFAC model are emphasised in this review. Challenges, future prospects and potential research directions are also provided. Following the introduction to pre-combustion capture technology in Section 2, important worldwide research progress, pilot plants and commercial facilities of pre-combustion carbon capture are presented in Section 3. Section 4 provides overview of carbon dioxide separation technologies for pre-combustion carbon capture. Moreover, reviews of ionic liquid in carbon capture and storage (CCS) and solubility model for carbon capture optimisation (with further emphasis on the IL-based UNIFAC model) are presented in Sections 5 and 6. This is followed by the summary of research gaps (Section 7), overview of challenges of pre-combustion carbon capture (Section 8), future prospects of pre-combustion carbon capture (Section 9) and conclusion (Section 10).
2. Introduction to pre-combustion carbon capture technology Pre-combustion carbon capture involves sequestration of carbon dioxide from fossil fuel or biomass fuel prior to completion of combustion process [46]. Its generic configuration is illustrated in Fig. 3. Typically, it is applied in (coal, natural gas and biomass) gasification and natural gas power plants [47]. A typical pre-combustion carbon capture system for gasification power plant, as depicted in Fig. 4, begins with gasification (or partial oxidation) of fuel to produce synthesis gas (or syngas) enriched with carbon monoxide and hydrogen. After particulate removal via cyclone separation unit, syngas is then processed in water gas shift (WGS) reformer wherein carbon monoxide reacts with steam to form carbon dioxide and hydrogen, and the resulted product stream is sent for desulphurisation and carbon dioxide separation
[44]. Ultimately, this carbon capture system generates hydrogen fuel stream for various power generation applications (i.e. gas boiler, gas turbine, fuel cell, etc.) with minimal sulphur dioxide generation, therefore raising the value of fuel by carbon content reduction [48]. Whereas in natural gas power plant, carbon dioxide separation unit is typically preceded by autothermal (steam) reforming and WGS processes [49]. Pre-combustion capture is often associated with process stream with higher carbon dioxide concentration (i.e. 15–60% by volume, dry basis), elevated pressure (i.e. 2–7 MPa) [51], and high temperature range of 200–400 °C [52]. Generally, the syngas stream after the catalysed WGS process has been reported to contain 64–73 mol % hydrogen and 20–23 mol% carbon dioxide [52]. High carbon dioxide partial pressure [48] in particular has thermodynamically driven the carbon dioxide adsorption with greater efficiency, and resulted in a lower energy demand for carbon capture and compression operation as compared to the post-combustion capture approach.
3. Important global research progress, pilot plants and commercial facilities 3.1. Pre-combustion capture research progress This section aims to review the research progress for precombustion carbon capture development worldwide. To date various research and development (R&D) works have been conducted to enhance the technological maturity and feasibility of precombustion capture technology. Significant research advances have been observed in the carbon separation technology development. Both simulation-based and experimental approaches were applied separately, or hand-inhand in these research works. Based on the literature research, adsorption, absorption, clathrate hydrate and membrane technology developments have been found to dominate the precombustion capture research domain. As shown in Fig. 5, adsorption technology has, inter alia, shown the most significant growth from 2009 to 2016. The references of reviewed literatures are presented in Table 4. Several transition trends have been noticed from the review. Firstly, for adsorption technology, the research focus evolves to novel/ modified materials (i.e. azo-linked polymer (ALP) [261], amine-modified titanium oxide [242], calcium oxide-based hollow sphere [250], melamine-modified phenol formaldehyde [257], mannitol-based ketal-linked porous organic polymer (MKPOP)
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 2 Summary of commercial post-combustion facilities worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Prosint Produtos Sintéticos, methanol production plant (Rio de Janeiro, Brazil)
Operating since 1967
90
Fluor’s Econamine FG Plus Process
Food-grade CO2 production
Rao et al. [25]
Kerr-McGee’s soda ash plant (Trona, California, USA)
Operating since 1978
800
Kerr-McGee/ABB Lummus Crest Process
Production of soda ash and liquid CO2
Barchas [26]
Lubbuck natural gas processing facility (Texas, USA) Indo Gulf Corporation Ltd, fertiliser plant (Jagdishpur, India)
1982–1984
1200
Fluor’s Econamine FG Plus Process
Operating since 1988
150
Enhanced oil recovery (EOR) application Urea production
Abu-Zahra et al. [27] Global CCS Institute [28]
300 MW coal-fired cogeneration plant (Poteau, Oklahoma, USA) Soda Ash Botswana soda ash facility
Operating since 1991
200
Food-grade CO2 production
Rao, Rubin [25]
Operating since 1991
300
Kerr-McGee/ABB Lummus Crest Process
Bellingham natural gas combined cycle power plant (Massachusetts, USA) Sumitomo Chemicals (Chiba, Japan) Liquid Air Australia (Two plants)
1991–2005
330
Fluor’s Econamine FG Plus Process
Operating since 1994 Operating since 1995
165 60
Production of food-grade CO2 for beverage production Food-grade CO2 production Food-grade CO2 production
Global CCS Institute [29] Rao, Rubin [25] Global CCS Institute [28]
Statoil’s Sleipner natural gas processing facility (Norway, North Sea)
Operating since 1996
2466
Amine scrubbing system
Oceanic storage at deep saline (Utsira) formation, 800–1000 meters below the sea bed
Global CCS Institute [30]
Petronas Fertiliser, steam reformer of fertiliser plant (Kedah, Malaysia)
Operating since 1999
160
MHI KM-CDR Process (using KS1 solvent)
Urea production
Iijima et al. [31]
Warrior Run 180 MWe coal-fired power plant (Cumberland, Maryland, USA)
Operating since 2000
330
Fluor’s Econamine FG Plus Process
Food processing, refrigeration and fire extinguisher production
Rao, Rubin [25]
Shady Point 320MWe coal-fired power plant (Oklahoma, USA)
Operating since 2001
800
Kerr-McGee/ABB Lummus Crest Process
Food and beverage processing, freezing and chilling purposes
Dooley et al. [32]
Chemical company, natural gas and oil-fired boiler (Kyushu, Japan) IFFCO/AONLA fertiliser plant (Aonla, India) IFFCO/PHULPUR fertiliser plant (Phulpur, India) Nagarjuna Fertilisers & Chemicals Ltd (Kakinada, India) Gulf Petrochemical Industries Company (GPIC) (Sitra, Bahrain) Ruwais Fertiliser Industries, natural gas reformer (Abu Dhabi, United Arab Emirate) Vietsovpetro White Tiger Project, Pyu-My 4000MW gas turbine combined cycle power plant (Pyu-My, Vietnam) Engro Chemical Pakistan Limited (ECPL), urea fertiliser plant (Pakistan)
Operating since 2005
330
General use product
Operating since 2006 Operating since 2009
450 450 450
MHI KM-CDR Process (using KS1 solvent)
Tatsumi et al. [33] Bandyopadhyay [34] Baron [35]
Operating since 2009
450
Urea and methanol production
Operating since 2009
400
Urea production
Operating since 2010
240
Operating since 2011
340
Enhanced oil recovery (EOR)/ enhanced gas recovery (EGR) application Urea production
National Fertiliser Ltd, Vijaipur plant (Madhya Pradesh, India)
Operating since 2012
450
Urea production
Qatar Fuel Additives Co. Ltd (QAFAC), methanol plant (Mesaieed, Qatar)
Operating since 2014
500
Methanol synthesis (yield enhancement)
Petra Nova Carbon Capture and Storage (CCS) Project, W. A. Parish coal-fired power plant (Texas, USA)
Under construction, operational by fourth quarter of 2016
4776
EOR at mature West Ranch Oil Field (Texas, USA)
Saskpower’s Boundary Dam Power Station (Saskatchewan, Canada)
Operating since 2014
2740
Cansolv Technology Inc. CO2 Capture Process
EOR at Weyburn Oil Field
MIT [40]
ROAD CCS Project, 1GW coal-fired power plant (Rotterdam, The Netherlands) Peterhead Project, 385 MW combined gas cycle turbine power plant (Scotland, United Kingdom) Bow City Power CCS Project, 1000 MW supercritical coal-fired power plant (Alberta, USA)
Under construction, operational by 2017 Under construction, operational by 2019
3014
N/A
Storage at depleted gas reservoir
MIT [41]
2740
Cansolv Technology Inc. CO2 Capture Process
Offshore storage at Goldeneye gas reservoir
Operational by third quarter of 2011
2740
Soda ash production
Production of urea, NPK, DAP, and NP Urea/ammonia production
Tatsumi, Yagi [33] Bandyopadhyay [34] Baron [35]
Mitsubishi Heavy Industries Ltd [36] Mitsubishi Heavy Industries Ltd [37] Mitsubishi Heavy Industries Ltd [38] Kamijo [39]
EOR
(continued on next page)
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Table 2 (continued) Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Shengli Oil Field EOR Project, Sinopec Qilu No.2 fertiliser plant (Shandong, China) Taweelah Project, natural gas-based TAPCO and EMAL power plants (Abu Dhabi, United Arab Emirates)
Operational by 2017
2740
N/A
EOR in Shandong Province
Operational by 2018
5479
N/A
EOR
Table 3 Summary of commercial pre-combustion facilities worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Pre-combustion capture plants Hydrogen Energy California Project, Hydrogen/petroleum coke-fuelled integrated gasification combined cycle (IGCC) power plant (California, USA) Texas Clean Energy Project, Coal-fired power plant (Texas, USA)
Constructed in 2015 and operational by 2020 Operational by 2019
8219
Onshore enhanced oil recovery (EOR) at Occidental’s Elk Hills Oil Field EOR at Bermian Basin
MIT [41]
Kemper County IGCC, Pre-combustion IGCC plant (Mississippi, USA)
Operational by 2016
9589
Rectisol AGR system Rectisol AGR system TRIGTM Technology
Killingholme Project, IGCC power plant (North Lincolnshire, United Kingdom) Don Valley Power Project, Coal-fuelled IGCC power plant (South Yolkshire, United Kingdom)
Operational by 2019
6849
Constructed in 2013 and operational by 2019 Constructed in 2013 and operational by 2015 Operational by 2020
13,425
Operational by 2015
Dongguan Project, Coal-fired 800 MW IGCC power plant (Dongguan, China) Huaneng GreenGen Project, Coal-fired 400 MW IGCC power plant (Bohai Rim, China) Lianyungang Project, Coal-fired 1200 MW IGCC power plant (Jiangsu, China)
5479– 8219
Onshore EOR
Selexol process Selexol process
Storage at deep saline formation
2740
TRIGTM Technology
EOR in Shandong Province
5479
N/A
EOR
2740
N/A
Oceanic storage at Binhai and EOR at North Jiangsu Oil Field
MIT [41]
Offshore storage at deep saline formation
Carbon Dioxide Storage Fuel
Carbon Dioxide Separation
Air
Exhaust Gas Fuel Combustion Heat & Power Fig. 3. Schematic diagram of pre-combustion carbon capture system [44].
[357], aramid [309], amine-modified molecularly imprinted polymer (MIP) [358], amine-impregnated silica nanotube [319], heterometallic MOF [318], multi-functionalised polymer [248], and multi-functionalised MOF [320]), composite materials (i.e. cadmium oxide/alkali metal halide mixture [135,179,244], hydrotalcite/graphene oxide composite [251], hydrotalcite/activated carbon composite [263], and metal oxyhydroxide/biochar composite [305]), and sustainable raw ingredients (i.e. mine waste [307], rice straw [247], and chitosan-based nano-composite [310]). Similarly, membrane-based research has also transitioned from single material exploration to composite membrane development [279,337,359], hybrid membrane contactor system [338,340], and mixed matrix membrane [283,339,341,342,360] for improved
performance. For clathrate hydrate separation process, different thermodynamic promoters (i.e. cyclopentane [58], tetra-n-butyl ammonium bromide (TBAB) [219], tetra-n-butyl ammonium chloride (TBAC) [295], tetra-n-butyl ammonium nitrate (TBANO3) [220], tetra-n-butyl ammonium fluoride (TBAF) [151], glucoamylase aqueous solution [347], and their mixtures [94]) and contact media (i.e. silica sand, water-saturated silica gel [74], cooled silica gel [158], glass bead [297], brine-saturated silica gel [196], metallic packing [291,294], alumina [223], coal bed [348,356], and waterin-oil emulsion [221]) have been tested. For absorption technology, the mainstream investigations have mainly dwelled in development and performance enhancement of solvents from 2011 to 2016, whereby the latest works have seen
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Syngas
CO2 Storage
CO2, H2
Fuel Steam Oxygen Cyclone Air Gasifier
Air Separation Unit (ASU)
Desulphurisation Column
CO2 Separator
Water Gas Shift (WGS) Nitrogen
Slag
Ash
Sulphur Exhaust Hydrogen Gas Turbine Air
Heat & Power
Fig. 4. Process flow diagram of pre-combustion carbon capture system for gasification power plant [50].
Table 4 References of reviewed pre-combustion capture research works.
Number of Published Research
45 40 35
Year
Carbon capture technology
Number of research
Refs.
30
2009
Adsorption Absorption Membrane Clathrate hydrate Hybrid
3 – 1 3 6
[53–55] – [56] [57–59] [60–65]
2010
Adsorption Absorption Membrane Clathrate hydrate Hybrid
5 – 2 4 1
[66–70] – [71,72] [73–76] [77]
2011
Adsorption Absorption Membrane Clathrate hydrate Hybrid
9 2 2 5 7
[78–86] [87,88] [89,90] [91–95] [96–103]
2012
Adsorption Absorption Membrane Clathrate hydrate Hybrid
11 2 6 6 4
[104–114] [50,115] [116–121] [122–127] [128–131]
2013
Adsorption Absorption Membrane Clathrate hydrate Hybrid
14 1 3 13 4
[132–145] [146] [147–149] [150–162] [163–166]
2014
Adsorption Absorption Membrane Clathrate hydrate Hybrid
42 2 6 9 15
[167–208] [209,210] [211–216] [196,217–224] [225–239]
2015
Adsorption Absorption Membrane Clathrate hydrate Hybrid
31 8 12 9 3
[240–270] [271–278] [279–290] [291–299] [300–302]
2016
Adsorption Absorption Membrane Clathrate hydrate Hybrid
27 5 8 10 6
[303–329] [330–334] [335–342] [46,343–351] [329,352–356]
Adsorption
25
Absorption
20
Membrane
15
Clathrate Hydrate
10
Hybrid
5 0 2009 2010 2011 2012 2013 2014 2015 2016
Year Fig. 5. Trend of pre-combustion capture research from 2009 to 2016.
the formulation of pure ionic liquid [331], hydrophobic physical solvent [332] and PEG-ionic liquid solvent blend [330]. Moreover, in recent years, with abundance of thermodynamics, kinetics, phase equilibria and cost databases, techno-economic and thermodynamic evaluations via simulations have gained popularity as pre-feasibility analyses prior to pilot and demonstration plant implementation [332,333]. It shall be noted that in contrast to other separation technologies lower number of published research in absorption is attributed to its transition to technology maturity phase, wherein the research communities are currently more engaged in implementing the pilot, demonstration and industrial-scale plants. 3.2. Pilot plant overview In tandem with the continuous research progress, many pilot testing programmes were carried out globally. Specifically, Vattenfall Group conducted a large-scale pre-combustion carbon capture validation programme prior to operation of commercial IGCC carbon capture plant in Buggenum, Netherlands. The purpose of this pilot testing is to obtain operational experience for coping with full-scale facility, verify the performance level of novel technology,
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and identify potential risks and mitigation measures. From the pilot testing, optimal system configuration, catalyst, solvent, construction material, upscaling strategy, and corrosion countermeasure were identified [361]. In Spain, ELCOGAS conducted pilot testing for examining the feasibility of pre-combustion carbon capture at Puertollano IGCC plant with hydrogen fuel synthesis, generating financial data for further upscaling purpose, increasing carbon dioxide recovery rate and reducing the carbon capture expenditure. The pilot plant research had demonstrated the technical and financial feasibility of upscaling the new technology to full scale (i.e. capacity of the existing gasification plant), and verified the operational robustness of pressure swing adsorption (PSA) technology [362]. Another successful pre-combustion carbon capture pilot study was implemented in the United States by Tampa Electric Company (TECO) in collaboration with the United States Department of Energy. In this pilot test, carbon dioxide solvency in amino acid salt formulation was examined while verifying the technical feasibility of novel technology anticipated to reduce the gasification plant operational cost [363]. Table 5 summarises the details of these pilot plant testing programmes. 3.3. Commercial scale plant overview In tandem with this research progress, many commercial scale pre-combustion carbon capture facilities have been built and operated worldwide. However, due to technological and financial constraints, physical absorption process still remains the most practical solution. Some of the commercial pre-combustion capture plants already in operational phase shall be discussed in detail as follows. Situated in Southwestern Kemper County, the Kemper County IGCC project consists of transport integrated gasification (TRIG) technology for fuel gas synthesis as feed to its combined cycle power generation system [364]. With TRIG technology, it could reportedly process 4.5 million tonnes per annum of low-quality lignite to produce synthesis gas sufficient for net power generation up to 524 MW [365]. The carbon capture facility of this project is based on physical absorption technology utilising Selexol process, which is able to reduce the carbon dioxide emissions by 67% with simultaneous synthesis of sulphuric acid (i.e. 135,000 tonnes per year) and ammonia (i.e. 20,000 tonnes per year) [366]. Another pre-combustion carbon capture facility that involves TRIG coal gasification process shall be featured by Dongguan Taiyangzhou IGCC power plant in Guangdong, China [367]. Being owned and operated by Dongguan Tian Ming Electric Power Co. Ltd. (TMEP), this 800 MW power generation facility is coupled with a cryogenic separation-based carbon capture facility with a capacity of 1 million tonnes per year. The captured carbon dioxide would be transported to off-shore gas/oil reservoirs for enhanced gas/oil recovery [41]. In Jiangsu, China, Lianyungang IGCC power plant
has also been constructed and operated by 2015 with a one-mil lion-tonne-per-year-capacity pre-combustion CCS system. Similarly, the captured carbon dioxide is transported via on-shore pipeline to the Northern Jiangsu oil-fields for enhanced oil recovery [41]. Table 6 shows the details of some commercial precombustion capture projects worldwide, all of which applying physical absorption technology. 4. Carbon dioxide separation technologies for pre-combustion carbon capture Typical carbon dioxide separation technologies for precombustion capture include physical absorption, adsorption, membrane, and cryogenic separation [20]. Each of these technologies is reviewed as follows. 4.1. Physical absorption technology Physical absorption technology includes two parts i.e. absorption and stripping processes, whereby in the former treated gas is contacted counter-currently with solvent stream and carbon dioxide is physically captured by the solvent whereas in the latter the carbon dioxide-saturated solvent is heated to regenerate the fresh solvent (to be recycled back to the absorption column) and release carbon dioxide at the top of stripping column (as illustrated in Fig. 6) [368]. Unlike the chemical solvents, extent of carbon dioxide absorption in the physical solvent is based on Henry’s law, i.e. linearly proportional to the partial pressure of carbon dioxide [370]. Without alteration of chemical identities of carbon dioxide and solvent [371], the dissolution of carbon dioxide in the liquid solvent is attributed to the van der Waals or electrostatic interaction between them, either of which being weaker than the chemical bonding as in the case of chemical absorption. Generally, physical absorption is optimal at high pressure and low temperature, while low pressure and high temperature conditions favour physical desorption [372]. With such pressure dependence of solvent loading, physical absorbent has better absorption performance than chemical absorbent at high partial pressure of carbon dioxide, while its regeneration could be easily achieved through depressurisation operation with lower energy demand (as compared to chemical absorption process) [44]. Therefore, it is more commonly used in precombustion carbon capture scenario, i.e. removal of carbon dioxide from synthesis gas as in IGCC power plants [361], natural gas treatment [48], as well as acid gas recovery (AGR) in coal or heavy oilfuelled chemical production processes (i.e. methanol, hydrogen, ammonia, substitute natural gas (SNG) and Fischer-Tropsch products) [370]. However, the absorption capacity of physical absorbent is only satisfactory at low temperature, therefore necessitating
Table 5 Details of pre-combustion carbon capture pilot plants worldwide. Pilot plant
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Puertollano, Coal and petroleum coke-fuelled integrated gasification combined cycle (IGCC) power plant (Puertollano, Spain)
Operational since 2010
100
Chemical absorption technology (using active methyl diethanol amine, aMDEA)
Recycled to IGCC process
Casero et al. [362]
Buggenum, coal and biomass-fuelled 253 MW IGCC power plant (Buggenum, The Netherlands)
Operational since 2011
34
Physical absorption technology (using dimethyl ether of polyethylene glycol)
Recycled to IGCC process
Damen et al. [361]
Polk Station, Coal-fuelled 250 MW IGCC power plant (Florida, USA)
Operational since 2014
822
Chemical absorption (Siemens POSTCAP Technology)
Storage at Lawson deep saline formation
Tampa Electric [363]
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 6 Summary of pre-combustion capture-based commercial-scale carbon capture plants worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Hydrogen Energy California Project, Hydrogen/petroleum cokefuelled integrated gasification combined cycle (IGCC) power plant (California, USA) Texas Clean Energy Project, Coal-fuelled IGCC power plant (Texas, USA) Kemper County IGCC, Pre-combustion IGCC plant (Mississippi, USA)
Constructed in 2015 and operational by 2020 Operational by 2019
8219
Rectisol AGR systema
MIT [41]
Operational by 2016
5479– 8219 9589
Rectisol AGR system TRIGTM Technologyb; Selexol process
Onshore enhanced oil recovery (EOR) at Occidental’s Elk Hills Oil Field EOR at Bermian Basin
Nuon Magnum, Multi-fuel 1200 MW (coal, biomass and natural gas) power plant (Eemshaven, The Netherlands)
Operational by 2020
N/A
Selexol processc
Storage at North Sea Oil and Gas Fields
Damen et al. [361]
Killingholme Project, IGCC power plant (North Lincolnshire, United Kingdom) Don Valley Power Project, Coal-fuelled IGCC power plant (South Yolkshire, United Kingdom)
Operational by 2019
6849
Selexol process
MIT [41]
Constructed in 2013 and operational by 2019 Constructed in 2013 and operational by 2015 Operational by 2020
13,425
Selexol process
Storage at deep saline formation Offshore storage at deep saline formation
2740
TRIGTM Technology
EOR in Shandong Province
5479
N/A
EOR
Operational by 2015
2740
N/A
Oceanic storage at Binhai and EOR at North Jiangsu Oil Field
Dongguan Project, Coal-fired 800 MW IGCC power plant (Dongguan, China) Huaneng GreenGen Project, Coal-fuelled 400 MW IGCC power plant (Bohai Rim, China) Lianyungang Project, coal-fuelled 1200 MW IGCC power plant (Jiangsu, China)
Onshore EOR
a Rectisol AGR System is a patented pre-combustion carbon capture method developed by Linde and Lurgi. It is a cryogenic acid gas removal (AGR) process that applies methanol as solvent. b Transport Integrated Gasification (TRIGTM) technology is a cleaner and more economical coal-gasification method co-developed by Southern Company, KBR and Department of Environment (DOE) of the United States [41], due to its ability for efficient low-ranked coal utilisation. c Selexol process is a bulk carbon dioxide absorption technique that applies a mixture of dimethyl ether polyethylene glycols as solvent [361].
CO2 Clean Gas Condenser
Cooler
Absorber Column
Flue Gas
Lean Solvent
Stripper Column
Rich Solvent
Lean-Rich Solvent Heat Exchanger Reboiler
Pump
Pump Fig. 6. Simplified schematic diagram of absorption-stripping process [369].
the cooling of treated gas stream prior to absorption process and lowering the overall process energy efficiency [373]. The established commercial physical absorption processes include Selexol, Rectisol, Purisol [44], Morphysorb and Fluor processes [370]. While their solvent types and vendors are as summarised in Table 7, the advantages and disadvantages of these patented physical absorption processes are compared in Table 8.
Meanwhile, ILs comprise another class of novel physical solvents. They are a class of salts with melting points below room temperature and therefore exist in liquid phase at room temperature [383]. This is attributed to the weak coordination and ionic bonding between the ionic species, especially when bulky and asymmetrically configured organic cations are bonded with organic or inorganic anions [384].
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Table 7 Chemicals and vendors of different commercial physical absorption processes. Process Selexol process
c d e f
Dimethyl ether of polyethylene glycol (DMPEG) a
Purisol process
N-methyl-2-pyrolidone (NMP)a Morpholine
Operating conditions
Union Carbide (United States)
a
3.59 MPa and 35 °Cc
a
Methanol
Fluor process a
Vendor a
Rectisol Process
Morphysorb process
b
Chemical
3.6 MPa and 25°Cd
Lurgi and Linde (Germany) ; Lotepro Corporation (United States)a
b
Lurgi (Germany)a
15 to 0 °C and 6.8 MPae
Gas Technology Institute (GTI) (United States) b
Propylene carbonate
Fluor Daniel, Inc.
b
b
6.9 MPa and 48.8 °Cf 2.72–5.78 MPa and 25 °Ce
Thambimuthu et al. [44]. Jansen et al. [370]. Kapetaki et al. [374]. Sadegh-Vaziri et al. [375]. Spigarelli [376]. Gas Technology Institute [377].
Table 8 Advantages and disadvantages of different commercial physical absorption processes. Physical absorption process
Advantages
Disadvantages
Selexol process
High selectivity for H2S Does not require water wash for solvent recovery Chemically and thermally stable Low volatility (i.e. minimal solvent loss) Flexible i.e. compatible with combined removal of H2S and CO2, and specific H2S removal [370] Capable of moisture removal (due to hydrophilicity of solvent) Minimal capital and operational expenditures (i.e. carbon steel construction) [378]
High viscosity at low side of operational temperature (i.e. 0–175 °C), with reduced mass transfer rate and tray efficiency [275] Only suitable for CO2 removal if CO2 is more concentrated than H2S [378]
Rectisol process
Good CO2 and H2S removal efficiency (i.e. <0.1 ppm) to avoid catalyst poisoning (suitable for synthesis of methanol, hydrogen, ammonia, synthetic natural gas (SNG) and Fischer Tropsch products) Enable simultaneous capture of H2S and CO2 Reasonable viscosity of solvent Minimal solvent loss [370] Lower energy demand than amine-based absorption processes Minimal foaming and good miscibility with water High thermal and chemical stability Low corrosivity Minimal solvent degradation [378]
Low temperature operation (i.e. 30 to 80 °C) [379], requiring expensive and complicated cryogenic process stages Possibility of amalgam formation (due to absorption of mercury) at low temperature [378]
Purisol process
High selectivity for H2S Flexible i.e. compatible with combined removal of H2S and CO2, and specific H2S removal [370]
Volatile solvent and requirement of water scrubbing to avoid excessive solvent loss [370]
Morphysorb process
High solvent loading capacity Selective removal of H2S and CO2 Reduced corrosion Reduced environmental hazard Low capital and operating costs [380] Lower energy requirement [381] Lower recirculation requirement Lower co-absorption of hydrocarbon [382]
Relatively new process with low maturity level (i.e. at laboratory trial and pilot testing stages) [381]
Fluor process
Non-corrosive and low viscosity solvent Enable selective removal of H2S High solubility of carbon dioxide No requirement of make-up water [378]
Uneconomical to achieve high product purity Requirement of cryogenic operational condition Requirement of more efficient gas-liquid contactor [373] High solvent recirculation requirement Expensive solvent [378]
The potential of these novel solvents has been recognised due to their low volatility, non-flammable, and recyclable natures [385]. Apart from that, they are preferred over the conventional organic solvents for their enhanced solvation potential for a wide range of organic and inorganic solutes [386], high thermal stability [387], and wide liquid range [388]. Besides, their adjustable solvent (i.e. physiochemical) properties based on the choice of constituting cations and anions [384] endow them the designation of ‘designer solvents’. However, for (non-functionalised) physical ILs, carbon dioxide solubilisation mechanism could be attributed to the Lewis acid-
base interaction between carbon dioxide (i.e. Lewis acid) and anions (i.e. Lewis bases) [389], solvent free volume and van der Waals interaction [390]. In the first mechanism, cation adjustment has seen auxiliary effect on the improvement of the carbon dioxide solubility, and imidazolium-based ILs are the most widely investigated and applied ones. In particular, Almantariotis et al. [391] found that the carbon dioxide solubility would increase with larger alkyl group of imidazolium (IM) cation, and more significantly fluorination of cation. Despite the reported significant affinity of imidazolium cation-based ILs towards carbon dioxide, other cations i.e. choline (CHO) [392], ammonium (N) [393], pyrrolidium (PYRR)
W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663
[394], pyridinium (PYR) [395], guanidinium (GUA) [396], piperidinium (PIP) [397] and phosphonium (P) [398] had also been investigated. Manipulation of IL anionic constituent would impose much more significant effect on its absorption capacity for carbon dioxide. In an experimental research by Aki et al. [399], carbon dioxide solubility was probed for different anions coupled with imidazolium cation, and it was found that the solubility increased in the order of nitrate (NO3) < dicyanamide (DCA) < tetrafluoroborate (BF4) < hexafluorophosphate (PF6) < triflate (TfO) < bis(trifluorome thylsulphonyl)imide (Tf2N) < methide anion. The increasing solubility trend is attributed to the increment in excess enthalpy of dissolution, which is primarily and secondarily contributed by the attractive van der Waals interaction and electrostatic bonding respectively. Despite their advantages over the conventional physical solvents, these ILs are still not ready for commercial-scale application due to its high viscosity and limited diffusivity, which could lead to unsatisfactory gas-liquid mass transfer (i.e. slow absorption rate) in the conventional absorption packed column [400]. Moreover, their prohibitively high costs have made it infeasible for absorption application in commercial-scale CCS facilities [401]. 4.2. Adsorption technology In contrast to the absorption process, adsorption involves selective formation of physical or chemical bonds between the carbon dioxide (adsorbate) and solid-phase adsorbent surface until the latter becomes saturated. Subsequently, adsorbed carbon dioxide is then desorbed through pressure swinging (as in pressureswing adsorption (PSA)) or temperature swinging (as in temperature-swing adsorption (TSA)) to regenerate the adsorbent material [44]. Typical sorbent technology configuration is similar to that of absorption process (Fig. 5). In TSA the saturated adsorbent is heated (using hot air or steam) to the temperature range at which the physical or chemical bond is broken to release the adsorbed species whereas in PSA pressure is reduced to achieve the same effect. It shall be noted that the former is preferred if the carbon dioxide concentration is not significant, while the latter is more compatible for the scenario whereby the carbon dioxide partial pressure is high [402]. In practical point of view, PSA is more appealing due to its shorter temporal requirement for adsorbent regeneration, and compatible with the economic need of bulk separation at full commercial scale (i.e. minimal idling time of adsorption bed) [44]. Theoretically adsorption has been reported to be superior in terms of high loading capacity at ambient conditions, less energy intensive and economical regeneration process, mechanical and chemical stability, high adsorption rate, simple operation and maintenance, and satisfactory tolerance with moisture and impurities in the flue gas [403]. Common physical adsorbents include activated carbon, zeolite [404], carbon molecular sieves, silica membrane and metal-organic framework materials (MOF) [405], whereas chemical adsorbents encompass calcium oxide (CaO), lithium metal-based sorbents and solid amine sorbents [404]. The technical details of these physical and chemical adsorbents are as summarised in Tables 9. 4.3. Membrane technology Membrane separation is a transport process based on Knudsen diffusion principle whereby the permeate (i.e. carbon dioxide) would dissolve in the membrane and diffuses through it at the rate proportional to its partial pressure gradient across the membrane [426]. According to Thambimuthu et al. [44], application of nonfacilitated membrane separation technology is more common to
1643
the carbon dioxide removal from natural gas (as in gas treatment process) and pre-combustion capture, whereby the carbon dioxide partial pressure is much higher. The proposed scheme of zero emission power plant utilising membrane technology is shown in Fig. 7. For the case of carbon capture from flue gas, since the carbon dioxide concentration is low, more energy penalty would be imposed (as compared to wet scrubbing process) due to requirement of compression work to ensure sufficient driving force for achieving the desired carbon capture ratio (CCR) and carbon dioxide purity [427]. Moreover, its selectivity could only be improved at cost of permeability, and vice versa [428]. Therefore, despite having advantages i.e. avoidance of steam utility, minimal environmental impact associated with solvent volatilisation and degradation, simple assimilation to the existing power plant [429], as well as design compactness and small footprint requirement [430], commercial application of membrane technology for postcombustion capture is still challenging. In view of such predicament, several alternative solutions have been introduced by the ongoing researches. One of the investigated alternative is facilitated transport membrane separation. It consists of mobile or fixed-site liquid phase carrier that enables active transport of carbon dioxide in the form of intermediate species i.e. bicarbonate. This would enhance the selectivity and permeability of carbon dioxide across the membrane [426]. Another class of modified membrane technology is constituted by mixed matrix membranes, which are polymer membranes impregnated with inorganic fillers [428]. The inorganic fillers tested include zeolite, carbon molecular sieve [431], MOF materials [430], zeolitic imidazolate framework (ZIF) materials [432], carbon nanotubes [433], titanosilicates and ordered mesoporous silica [434]. Such modification results in membrane with concurrent enhancement of selectivity and permeability, lower processing cost (due to polymer), better handing properties relative to inorganic membranes [428], good mechanical stability [431], better thermal stability and lower vulnerability to plasticisation (induced by high partial pressure of carbon dioxide) [435]. Gas membrane contactor (or hybrid membrane/solvent system) is another novel membrane-based separation technology gaining attention for development. In this system, separation is not based on Knudsen diffusion across the membrane but membrane only serves as a contacting medium between flue gas and carbon dioxide absorption solvent [426]. This modified technology exhibits the compactness of membrane system (and therefore lower capital cost), high selectivity (for carbon dioxide) of amine-based absorption process, and high flexibility for gas and liquid flow velocities [44], besides avoiding phase dispersion [426] and operational complications i.e. foaming and flooding [44]. The only disadvantage is the reduction of carbon dioxide mass transfer due to resistance imposed by the membrane framework [426]. 4.4. Cryogenic separation Cryogenic separation technology involves a series of cooling and compression operations at sub-ambient temperature and high pressure for separation of gaseous components in the carrier stream [436]. This technology has been widely used for production of high-purity liquid carbon dioxide (for food processing applications) and typically for pre-combustion captures process involving high carbon dioxide concentration (i.e. more than 90% by volume). Typical schematic diagram of cryogenic distillation unit is shown in Fig. 8. Cryogenic separation technology, in fact, overcomes some shortcomings of the conventional amine-based scrubbing process by avoiding excessive water consumption, need of expensive chemical agents, corrosion and foaming issues, need of winterisa-
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Table 9 Descriptions and comparisons of different physical adsorbents. Physical adsorbent
Description
Advantages
Disadvantages
Operating conditions
Activated carbon
Char material with high porosity, which could be activated physically or chemically; Physically activated carbon is formed via two (2)-stage process, i.e. pyrolysis of carbonaceous precursors at temperature below 800 °C to drive away volatile matters and form char, and activation of char with air/oxygen/steam/carbon dioxide; For chemical activation, precursors are first impregnated with dehydrating agent, followed by pyrolysis. Activation by chemical agent occurs simultaneously with charring process [403]
Suitable for low-temperature operation [404] High carbon dioxide capture capacity (of 10–15% by weight) due to highly porous structure/large adsorption surface area [404] Higher tolerance with water vapour [406] Inexpensive and low energy demand for regeneration [407] Long-term stability (i.e. negligible deactivation after 10 consecutive cycles) [407]
Lower selectivity for carbon dioxide over nitrogen than zeolite [407]
25 °C and 3 MPa [53]
Zeolite
Crystalline aluminosilicates with threedimensional framework enriched with cavities and channels through/in which small molecules, ions and entities may penetrate/ reside [408]
Suitable for low temperature operation [406] High loading capacity and selectivity for carbon dioxide [406] 5–10 times higher carbon dioxide/nitrogen selectivity than activated carbon [407]
Lower performance level when dealing with wet flue gas (because hydrophilic adsorption sites would be occupied) [406] Lower adsorption capacity [404]
0.72 MPa and 120– 200 °C [84]
Carbon molecular sieve
Special class of activated carbon with narrow pore distribution, engineered porosity, and capability of selective adsorption based on shape, size, adsorption rate difference, and discrepancy in adsorption equilibrium; Mainly made by controlled pyrolysis and carbon vapour deposition (CVD) techniques [405]
High tolerance with moisture content High resistance against corrosion by acids/alkalis High resistance against thermal degradation Higher selectivity for planar molecule (i.e. carbon dioxide) [405] Satisfactory permeability for carbon dioxide [409]
Costly and complicated manufacturing process (due to delicate nature of precursor material and risk of thermal expansion) [410]
5–35 °C and 0.1 MPa [411]
Mesoporous silica
Silica material with pore size between 2 and 50 mm, synthesised by reaction between soluble silica and surfactant template [412], organic template method in water/oil phase [413], and spray-drying of mixture of silica and polymer nanoparticles [414]
Large surface area for adsorption High capturing capacity (i.e. pore volume) Adjustable pore size High thermal and mechanical integrity [372] Low cost, harmless and chemically inert [413]
Not practical due to unsatisfactory carbon dioxide adsorption capacity at ambient pressure [372]
25 °C and 1– 3 MPa [415]
Metal-organic framework (MOF) material
Compounds assembled by metallic ions and organic ligands (containing nitrogen and oxygen elements), with one, two or threedimensional porous structure [416]
High surface area for adsorption Tunable pore structure and pore surface properties (via manipulation of metallic cation and ligand) High adsorption capacity at high pressure [372] High selectivity for carbon dioxide [416]
Performance level degradation due to presence of impurities (i.e. impractical) [372]
10 bar and 40 °C [417]
Calcium oxide (CaO)
CaO is used to chemically adsorb carbon dioxide in the form of calcium carbonate (CaCO3) at temperature greater than 600 °C in carbonation process; CaO could be regenerated via calcination at temperature above 900 °C [44]
High adsorption capacity High raw material availability Low cost of raw material [407] Established/long track record for industrial application Availability of high-level heat (from carbonation process) to be harnessed (i.e. for steam generation) and improve overall process energy efficiency [404] Durable and mechanically strong Fast adsorption/desorption rate [418]
Fast deactivation rate of calcium oxide and requirement of substantial replacement for practical operation [419]
650–950 °C, and 1– 42 bar [420]
Lithium-based adsorbent i.e. lithium silicate (Li4SiO4) and lithium zirconium (Li2ZrO3)
Chemical adsorption of carbon dioxide is elicited by the reversible reaction between lithium-based sorbent and carbon dioxide to form intermediates (i.e. for Li4SiO4, lithium carbonate (Li2CO3) and lithium metasilicate (Li2SiO3) [421]; for Li2ZrO3, Li2CO3 and zirconium oxide (ZrO2) [422] at temperature range of 500–700 °C; Adsorbent is regenerated by thermal decomposition of these intermediates
High capturing capacity Lower regeneration temperature compared to CaO (i.e. less than 750 °C) Sufficient adsorption/desorption rate High durability and stability (i.e. low performance decay rate) [421]
Low kinetics at high temperature (especially for Li4SiO4), requiring promoters to improve the performance [421] Expensive and difficult production due to scarcity and toxicity of raw materials [423]
400–600 °C and 1– 50 bar [424]
Amine-based sorbent
Solid support/nanoparticle/membrane with immobilised or impregnated amine solvent; The capture of carbon dioxide is based on the chemistry with amine
Low regeneration heat requirement (due to low heat capacity of solid sorbent) [372] High adsorption/desorption capacity Thermal stability at temperature up to 120 °C [404] Avoidance of corrosion problem High selectivity for carbon dioxide Proven tolerance with moisture content in flue gas [425]
Limited capture and regeneration efficiencies to make the process economically feasible [425] High cost [372]
25–85 °C and 0.1–1.0 CO2 partial pressure [241]
W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663
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Fig. 7. Proposed scheme of zero emission power plant utilising membrane carbon dioxide separation technology [44].
Fig. 8. Schematic diagram of cryogenic distillation unit [44].
tion modification [437], and pollution associated with emissions of solvent and degradation products [438]. This technology also offers the possibility of ambient pressure operation (i.e. avoiding associated hazards) and readily produces liquid carbon dioxide, therefore subsequently enabling economical carbon dioxide transportation [436]. Despite being one of the mature separation technologies, cryogenic separation process suffers several key problems. Firstly, due to operation at extremely low temperature (and high pressure), it
is very energy intensive (i.e. approximately 6–10 MJ per kg of recovered carbon dioxide) and therefore involves significantly high operational expenditure [20]. Moreover, possibility of ice formation in cryogenic process may lead to blockage of piping system and significant pressure drop, leading to possible equipment safety problem [439]. This necessitates the removal of moisture content prior to separation and therefore more financial investment on the required dehydration pre-treatment. In addition, frost (i.e. water and carbon dioxide) formed during operation may
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Table 10 Multi-faceted comparison of carbon dioxide separation technologies. Aspect
Physical absorption
Adsorption
Membrane technology
Cryogenic separation
Ref.
Technical advantages
Most established for precombustion carbon capture; Recoverable physical solvent from regeneration
Reversible process and recoverable adsorbent; High adsorption efficiency (of more than 85%)
Mature technology; Long track record for industrial carbon dioxide recovery
Leung et al. [20]
Technical disadvantages
Significant heat requirement for solvent regeneration; Absorption efficiency depends on carbon dioxide concentration; Possible environmental impacts from solvent degradation
Requirement of high temperature adsorbent; High energy requirement for carbon dioxide desorption
High commercial availability; High separation efficiency (of more than 80%) Operational issues i.e. low fluxes and fouling
Carbon dioxide separation yield (%) Energy Requirement (MJ/kg CO2)
90–98
80–95
80–90
>95
4.0–6.0
2.0–3.0
0.5–6.0
6.0–10.0
accumulate around the heat exchanger, increasing undesirable insulation and decreasing the heat transfer efficiency [436]. 4.5. Comparison of CO2 separation technology The technical advantages and disadvantages, carbon dioxide separation yield, energy requirement, environmental impact and financial aspect of the carbon dioxide separation technologies discussed above are summarised in Table 10. 5. Ionic liquid in carbon capture and storage (CCS) As mentioned in Section 3, physical absorption remains the most practical solution among the carbon dioxide separation technologies. Apart from the existing conventional physical solvents, the research community is still in a frenzy venture of discovering new pure solvents and solvent blend formulations with better properties. Among these experimental trials, ILs have stood out as a popular agenda due to their tunable solvent characteristics, thermal stability, minimum volatile loss, and reduced degradation-related emissions. This section reviews the IL-based carbon capture research and development. Main research scopes for IL-based carbon capture application comprise of biogas/natural gas upgrading as well as carbon capture at heat and power generation sites. For each scope, IL-based carbon separation technology development, optimisation, and techno-economic analysis for potential commercial facilities have been conducted. Specifically, for absorption-based biogas upgrading process, García-Gutiérrez et al. [440] had conducted techno-economical assessment on physical absorption-based biogas upgrading process using 1-ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [emim][Tf2N], 1-hexyl-3methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [hmim] [Tf2N] and trihexyl(tetradecyl)phosphonium bis[(trifluoromethyl) sulfonyl]imide [thtdp][Tf2N], and found that the costs of these facilities were in the range of USD 9.18-11.32/GJ (lower heating value) with overall efficiency of 71–86%. In another study concerning the optimisation of thermodynamics and mass transfer properties of IL-polyethylene glycol dimethyl ether (NHD) mixture for biogas upgrading purpose, Zhang et al. [441] found that the optimum composition with maximum carbon dioxide/ methane selectivity was 50 wt% IL and 50 wt% NHD. In a solvent screening investigation, Privalova [442] assessed the solvent performances of aqueous amine solutions, conven-
Only viable for high carbon dioxide concentration (i.e. more than 90% by volume); Sub-zero temperature requirement; Significant energy penalty
Mondal et al. [436]
tional ionic liquids, ‘switchable’ ionic liquids and poly(ionic liquid)s, and found 1-butyl-3-methylimidazolium acetate [bmim] [Ac] the most promising with high carbon capture efficiency and 65 wt% VOC elimination. Moreover, Xie et al. [443] had evaluated the energy performances of biogas upgrading processes using [bmim][Tf2N], [hmim][Tf2N] and 1-butyl-3-methylimidazolium hexafluorophosphate [bmim][PF6] via simulation studies, and found that [bmim][Tf2N] was associated with the lowest energy intensity with energy consumption 11% lower than the water scrubbing process. For novel IL-based separation technology development for biogas/ methane upgrading purpose, Hojniak [444] assessed the selectivity of supported IL membrane (SILM), and indicated that tri(ethylene glycol) and nitrile groupfunctionalised imidazolium and pyrrolidinium ILs had 2.3 times greater carbon dioxide/methane selectivity compared to those functionalised with glycol group only. Whereas Wang et al. [445] had developed an IL-tethered activated carbon granule for packed bed adsorption with adsorption capacity of 2.95 mmol/g, carbon dioxide/methane selectivity of 95% and high multi-cyclic stability at the optimal conditions of 0.5 MPa and 20 °C. In another study, Singh, Cowan [360] optimised the performance of poly(ionic liquid)-ionic liquid-zeolite mixed matrix membrane by manipulating zeolite particle type, zeolite particle loading, poly(ionic liquid) structure, quantity of crosslinking, and zeolite dispersion pattern. Similarly, Nayak [446] developed IL-immobilised Matrimid mixed matrix membrane to overcome instability of the conventional SILM in high pressure application, and found that incorporation of MOF i.e. Cu3(BTC)2 would increase its carbon dioxide and methane permeabilities to 240 and 843 barrer. Besides, Cheng et al. [447] evaluated the adsorption performance of molecular sieve impregnated with phosphonium-based IL for upgrading of biogas into vehicle fuel, wherein IL-loaded molecular sieve was found to exhibit greater carbon dioxide adsorption rates compared to the pure analogous IL in both pure carbon dioxide and biohythane atmospheres. For power plant carbon capture purpose, Gao et al. [273] had developed an IL-tailored amine aqueous solution comprising of 30 wt% N-methyldiethanolamine (MDEA), 3 wt% piperazine (PZ), 57 wt% water and 10 wt% butyl-3-methylimidazolium tetrafluoroborate [bmim][BF4] with reduced sensible heat, highest carbon dioxide solvency potential and lowest solvent regeneration enthalpy. In addition, Luo et al. [448] introduced a modified amino-functionalised IL with incorporation of N or O atom for carbon capture; this new solvent had reduced viscosity, greater mass transfer, and reduced column size requirement due to the
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formation of intra-molecular hydrogen bonding. Hydrophobic IL solvent i.e. allyl-pyridinium bis(trifluoromethylsulfonyl)imide was also synthesised by Siefert, Agarwal [332] for precombustion capture at IGCC plant with lower levelised cost of carbon capture (LCOC) compared to Selexol process. Apart from solvent development for absorption process, Otani et al. [449] had developed facilitated transport membrane (FTM) loaded with triethyl(methoxymethyl)phosphonium pyrrolide, which was found to have maximum reactivity with carbon dioxide and superior rheological property. While Li et al. [450] had developed stronger [bmim][Tf2N]-ZIF-8 filler material for the synthesis of mixed matrix membrane with enhanced tensile strength, carbon dioxide flux and selectivity, Ma et al. [451] incorporated aminebased task specific IL (TSIL) into MOF (i.e. NH2-MIL-101(Cr) to synthesise highly carbon dioxide selective mixed matrix membrane with improved carbon dioxide permeability (i.e. 2979 barrer). In a study for evaluating the potential of amino acid IL (AAIL) as carbon dioxide carrier in FTM, Kasahara et al. [452] found that AAIL with greater amino acid density increased the FTM carbon dioxide permeability and selectivity. Whereas Deng et al. [359] synthesised a composite membrane with incorporation of cellulose acetate (CA) and ether-functionalised pyridinium-based IL, with significant improvement in carbon dioxide permeability. In addition, Tengteng et al. [453] had synthesised SILM from PEG-200 and choline prolinate [Cho][Pro] for toxicity reduction and cost effectiveness enhancement. In terms of the development of supported ionic liquid phase (SILP), Pohako-Esko et al. [454] found that IL-modified chitosan ionogel (formed by dissolution of chitosan in IL) encapsulated with nanoporous fumed silica had exhibited improved carbon dioxide adsorption capacity while Gouveia et al. [455], from the assessment of the potential of cyano and amino acid-based IL mixtures for SILP synthesis, indicated that ILs with L-alanine and taurinate anions were associated with high carbon dioxide permeability and selectivity. Moreover, Styring et al. [456] had screened the optimal solid IL (SoIL) for pressure swing adsorption application via molecular simulation approach. In another study; in this analysis, SoIL was found to have high adsorption selectivity, moderate adsorption capacity, fast adsorption kinetics, low volatile loss and great thermal stability. Besides, Mahmood et al. [457] synthesised an IL polymer from 1-vinyl-3-ethylimidazolium bromide and 1-vinyl-3ethylimidazolium bis (trifluoromethyl-sulfonyl) imide, with incorporation of activated carbon; the resulted polymers had greater carbon dioxide adsorption capabilities due to combined actions of absorption and adsorption. Apart from that, Zhou et al. [458] had developed alpha zirconium phosphate (ZrP) and montmorillonite (MMT) hybrid inorganic nano-sheets incorporated with 1butyl-3-methylimidazolium chloride, which exhibited carbon adsorption capacities of 0.73 mmol/g and 0.42 mmol/g at the optimum operating temperatures of 60 and 70 °C. For more efficient carbon capture at power generation facility, Lu et al. [459] had developed a hybrid carbon capture technique coupling the membrane contactor and membrane vacuum regeneration. In this study, aqueous [bmim][BF4] and 1-(3-aminopropyl)-3-methyl-imi dazolium tetrafluoroborate [apmim][BF4] solutions were associated with the optimal water contents of 60 mol% and 40 mol%, and the latter was found to have greater carbon dioxide loading capacity while the former exhibited higher regenerability (at low vacuum degree). In a similar fashion, Dai et al. [338] evaluated the materials for the synthesis of porous and non-porous hollow fibre membranes loaded with 1-butyl-3-methylimidazolium tricyanomethanide, and selected porous PTFE membrane and nonporous Teflon-PP composite membrane for membrane reactor development. Both materials had comparable mass transfer performance, while the latter exhibited greater stability during operation.
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Apart from the carbon dioxide separation technology development, Valencia-Marquez et al. [460] had conducted a technoeconomic and dynamic analyses on an IL-based carbon capture pilot plant, and indicated that it had lower energy demand and could tolerate with fuel gas flow rate fluctuation by 10% with satisfaction of specified carbon dioxide recovery and purity requirements. Moreover, from the controllability analysis conducted on an IL-based pilot-scale carbon capture plant, Valencia-Marquez et al. [461] had developed and optimised an efficient and decentralised multi-loop control system for enhancing its economics, safety level, operational robustness and environmental sustainability.
6. Solvent design optimisation for pre-combustion carbon capture To date, many carbon capture plants based on pre-combustion capture configurations have been planned, constructed and prepared for steady-state operation. In the future, these carbon capture technologies would become even more important in order to mitigate the global warming effect (i.e. to achieve desirable 2C Scenario), provided the ever increasing carbon dioxide emissions from power generation and heavy industrial sectors. Physical absorption technology still remains dominant in the pre-combustion carbon capture sector, with established track records as well as numerous patented processes being commercialised worldwide [462]. As part of the carbon capture process optimisation, many ongoing researches have been directed to optimisation of solvent design, with the aim of formulating new solvents and solvent blends with optimal characteristics. For carbon capture purpose, these selection criteria encompass better absorption capacity and selectivity, easy desorption (i.e. lower regeneration heat requirement), higher thermal and chemical stabilities, greater resistance against oxidative degradation, lower volatility and solvent loss, and lower toxicity and environmental impacts [463]. Conventional solvent design approach is basically bottom-up, i.e. combination of physicochemical knowledge base, expert judgment and experience, and empirical trials (i.e. laboratory synthesis of solvent formulation and testing) [464]. These approaches first identify molecules from the raw materials, and then scrutinise the preferred properties from the identified molecules [465]. Since these approaches identify compatible solvent candidates via trialand-error manner, they are generally time-consuming, expensive, tedious and posing certain hazards to experimenters despite guaranteeing the accuracy and reliability of results. Screening of solvent through property database is another simple approach, but its effectiveness relies on the extensiveness and accuracy of existing database. Moreover, it is not time and cost-effective [466]. Computational thermodynamics is a more appealing approach. Known as computer aided molecular design (CAMD), it is defined as a reversed engineering approach that generates feasible molecules from the specified building blocks which meet the targeted chemical properties. In some way, this approach first translates the desirable chemical product attributes into measurable physical properties, and then design molecular structures with the identified properties under specified constraints [467]. CAMD is a more systematic and efficient way of designing promising candidate solvents from the existing fundamental building blocks and database, therefore narrowing the scope of combinatorial experimental solvent screening down to a few promising ones only as well as achieving significant saving in terms of time and cost. According to Gani [467], CAMD design framework consists of four main steps, namely problem formulation (i.e. specification of desirable solvent properties), initial search (i.e. preliminary
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identification of functional group/molecule compatible with identified pure component properties from the existing property database), generation of molecular structures (using appropriate CAMD techniques) and evaluation of their properties (benchmarked against desired ones specified in the first step), and verification (i.e. simulation of chemical process using the designed candidate). Therefore, property prediction models are very essential tools in CAMD, and the reliability of CAMD-based solvent design outcome largely depends on their accuracy and robustness. Among them, solubility model that accurately predicts the phase equilibrium of all components in the carbon capture system (i.e. gas stream and solvent stream) is of utmost importance, since it is related to other essential solvent attributes i.e. solvent loss, selectivity and solute distribution coefficient [466]. Therefore, there have been ongoing research and development works for improving the solubility model of carbon dioxide in various solvents and solvent blends. 6.1. Review of solubility models for carbon capture To date, numerous models have been developed for prediction of carbon dioxide solubility in various physical and chemical solvents, as well as solvent blends. For phase equilibrium modelling, both homogenous and heterogenous approaches are possible, whereby for the former equation of state (EOS) models are commonly applied whereas for the latter chemical potentials of gas and liquid phases are separately computed. While gas-phase chemical potential (i.e. fugacity coefficient) is usually calculated using EOS models, liquid-phase chemical potential (i.e. activity coefficient) evaluation models comprise of ab initio (first principle), semi-empirical and empirical models, as listed in Table 11. Their brief technical details are as summarised in Table 12. From the summary, it could be seen that recent development has been focusing on the prediction of carbon dioxide solubility in ILs due to its advantages over the conventional amine-based solvent formulations. The developed solubility models include quantum mechanics-based models (i.e. Conductor-like Screening Model
Table 11 Categorisation of models applied for prediction of carbon dioxide solubility in different solvents. Ab-initio model
Semi-empirical model
Empirical model
Conductor-like Screening Model for Real Solvents (COSMO-RS) Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC)
Modified UNIFAC (Dortmund)
Molecular dynamics simulation of Hildebrand’s solubility parameter
Electrolyte NRTL (E-NRTL) model
Modified Kent Eisenberg (MKE) model Quantitative structure-property relationship (QSPR) model Artificial neural network (ANN)
Non-random Twoliquid (NRTL) model
Debye-Huckel (DH) model Extended DebyeHuckel (EDH) model Pitzer model
Statistical Associating Fluid Theory (SAFT) variants Group Contribution (GC) Equation of State (EOS)
Multilayer perceptron network (MLP) Least square support vector machine (LSSVM) Adaptive neuro inference system (ANFIS) Committee machine intelligent system (CMIS)
for Real Solvents (COSMO-RS), Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC) and molecular dynamics simulation), semi-empirical models (i.e. modified UNIFAC (Dortmund) model, Group Contribution Equation of State (GC EOS), Perturbed Chain Hard Sphere (PCHS) model, and Soft Statistical Associating Fluid Theory (Soft-SAFT) model), and empirical model (i.e. Quantitative Structure-Property Relationship (QSPR) model). While COSMO-based models and statistical molecular models (i.e. SAFT EOS variants, GC EOS, lattice models, etc.) have been extensively developed for systematic screening of ILs for carbon capture purposes, limited work had been conducted in exploring the capability of UNIFAC model variants in prediction of carbon dioxide solubility in ILs. In particular, only UNIFAC model [498] and modified UNIFAC (Dortmund) model [482] were regressed for predicting solubility of carbon dioxide in ILs. Moreover, in these works, the IL-based solubility databases applied were much less extensive compared to those in COSMO-based model development, and only binary vapour-liquid equilibria (VLE) was investigated. COSMO-based models, despite requiring minimal experimental data due to its predominant dependence on quantum mechanical information of chemical species, were found to erroneously predict the carbon dioxide solubility trend [499]. Moreover, the optimisation of structural configuration of molecules/ionic systems (based on minimisation of potential energy) as well as quantum mechanical computation of surface charge density (in the form of sigma profile) is computationally extensive and complicated. Another much developed counterpart i.e. SAFT models involve complex formulations with numerous pure component parameters and cross-association binary parameters, and therefore limit its applications in engineering field [498]. On the other hand, group contribution model is simpler to apply and has received increasing attention due to its increasing assimilation in many commercial process design simulation software (i.e. Aspen Plus, Aspen Hysis, PROII, Chemcad, ROMeo and Dynsim). More detailed review of IL-based UNIFAC model is as presented in Section 3.2. 6.2. Review of ionic liquid (IL)-based UNIFAC model UNIFAC group contribution model is designed to predict the liquid-phase activity coefficient in non-ideal liquid mixture [500]. In any variant of the UNIFAC model, the activity coefficient of a compound in multi-component mixture is considered as the summation of all functional group activity coefficients, each arising from interaction of any two specific functional groups. These interactions result in combinatorial and residual group contributions to the overall molecular activity coefficients, whereby the former is attributed to the disparity in the molecular shapes and sizes of interacting structural groups and the latter by disparity in their molecular interaction types [501]. The combinatorial group contributions of functional groups to the activity coefficient was derived based on the Staverman potential as in UNIQUAC model [500], and involve group surface area (Q k ) and volume (Rk ) parameters. Whereas the residual group contributions, computed using the UNIQUAC residual term calculation method [500], are related to the group area fraction and parameter associated with group energetic interactions (wmn ). The group surface area, volume and interaction parameters for a massive number of structural groups were comprehensively reviewed and revised for improvement [502]. For UNIFAC models extended for IL solvent screening, there are three approaches for establishing the subgroups of ILs, as described as follows: Approach 1: This approach considers separation of each IL into a cation and an anion [503]. Since the substituents on each cationic species are not separated as subgroups, the impacts of their struc-
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 12 Summary of solubility models for prediction of carbon dioxide solubility in different solvents. Solvent type
Model (chemical potential calculation)
System type
Ref.
Binary vapour-liquid equilibrium (VLE) (C1 - C5 alcohols)
Hsieh et al. [468]
Gas-phase
Solvent-phase
Alcohols
Peng-Robinson-Stryjek-Vera (PRSV) equation of state (EOS)
Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC)
Alkanes
Homogenous approach Statistical Associating Fluid Theory for Potentials of Variable Range (SAFT-VR)
Ternary VLE (CO2 - methane - octane system)
Keskes et al. [469]
Amines
Soave-Redlich-Kwong (SRK) EOS
Quaternary VLE (mixture of three amines) Binary and ternary VLE (monoethanolamine (MEA), diethanolamine (DEA) and 2-amino-2methyl-1-propanol (AMP)) Binary VLE (MEA, DEA, AMP, methyl diethanolamine (MDEA), triisopropanolamine (TIPA) and 2amino-2-ethyl-1,3-propanediol (AEPD) ⁄ Include ionic species resulted from degradation of MEA; Ternary and quaternary VLE
Haghtalab and Ghahremani [470] Park et al. [471]
N/A
Peng Robinson (PR) EOS
Second-order virial equation
Electrolyte Non-random Twoliquid model (E-NRTL) Modified Kent-Eisenberg (M-KE) model
M-KE model; Extended Debye-Huckel (E-DH) model; Pitzer model NRTL model for molecular species; Debye-Huckel model for ionic species
Homogenous approach Electrolyte SAFT-HR (eSAFT-HR) Alternative Feed-forward multi-layer neural network model Alternative Multilayer perceptron network (MLP); Genetic algorithm - radial basis function network (GA-RBF); Coupled simulated annealing - least square support vector machine (CSA-LSSVM); Adaptive neuro inference system (ANFIS); Particle swarm optimisation - ANFIS (PSO-ANFIS); Committee machine intelligent system (CMIS)
Ternary VLE (Aqueous MDEA solution) Ternary/Quaternary/Higher VLE Quaternary VLE (aqueous mixture of MDEA and N-methylpyrrolidone (NMP))
Goharrokhi et al. [472]
Ostonen et al. [473]
Najafloo et al. [474] Hamzehie et al. [475] Tatar et al. [476]
Ester mixtures
Ideal gas assumption
Empirical EOS based on Hildebrand’s solubility parameter
Ternary VLE
Gui et al. [477]
Ionic liquids (IL)
SRK EOS
Conductor-like Screening Model for Real Solvents (COSMO-RS) COSMO-RS model
Binary VLE
Maiti [478]
Binary VLE; Estimation of Henry’s constants of CO2, nitrogen and methane in 2701 ILs Binary VLE; Estimation of Henry’s constants of CO2 in 13,356 ILs Binary VLE; Consider selectivity of CO2 over nitrogen, methane and hydrogen Binary VLE
Sumon and Henni [479]
Not relevant (i.e. Henry’s constant estimation)
Ideal gas assumption
COSMO-SAC model
Predictive SRK (PSRK) EOS
Modified UNIFAC (Dortmund)
Homogenous approach Perturbed Hard Sphere Chain (PHSC) EOS Homogenous approach Soft-SAFT Homogenous approach Group Contribution (GC) EOS Alternative Quantitative Structure-Property Relationship (QSPR) Alternative Molecular simulation of Hildebrand solubility parameters Polymers
Alternative QSPR
Electrolyte solutions/water
PRSV EOS
Electrolyte variant of UNIQUAC model
Homogenous approach Modified ion-based SAFT (SAFT2-KMSA) EOS Homogenous approach
Binary VLE Binary VLE (of CO2 and N2O in various ILs) Prediction of solubilities of CO2, CO, hydrogen, methane and ethane in [Cnmim][Tf2N] family ILs Binary VLE
Farahipour et al. [480] Lee and Lin [481]
Hizaddin et al. [482] Bazargani and Sabzi [483] Pereira et al. [484] Pereda et al. [485]
Eike et al. [486]
⁄Solubility parameters of CO2, methane, nitrogen, hydrogen, sulphur dioxide and nitrogen oxides in ILs
Sistla et al. [487]
Binary SVE (Polyethylene (PE), polypropylene (PP), polystyrene (PS), polyvinyl acetate (PVA) and poly (butylene succinate) (PBS))
Golzar et al. [488]
Binary VLE (CO2 and hydrogen sulphide in water and potassium carbonate) VLE of CO2 with single and mixed electrolyte solutions containing Na+, K+, Ca2+, Mg2+, Cl-, Br- and SO24 Quaternary VLE (CO2-water-hydrogen
Tang et al. [489] Jiang et al. [490]
Ji and Zhu [491] (continued on next page)
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Table 12 (continued) Solvent type
Model (chemical potential calculation) Gas-phase
System type
Ref.
Solvent-phase
Ion-based SAFT (SAFT2) EOS Homogenous approach Modified SAFT EOS with restricted primitive model (SAFT1-RPM) Homogenous approach Combination of Perturbed-Chain SAFT (PC-SAFT) EOS and Debye-Huckel term (ePC-SAFT) Homogenous approach PC-SAFT; Truncated PC-Polar SAFT (tPC-PSAFT) EOS Homogenous approach Extension of PPC-SAFT (ePPC-SAFT) EOS Homogenous approach Electrolyte-based extension of SAFT-VR (SAFT-VRE) EOS Homogenous approach SAFT-Lennard Jones (LJ) (SAFT-LJ) EOS
sulphide-sodium chloride) Binary (CO2-water) and ternary VLE (CO2-water-sodium chloride) VLE of CO2 and sulphur dioxide in brines at high pressures and temperatures Binary VLE of CO2 and water
Binary VLE (in 20 alkali-halide aqueous solutions) Binary VLE of CO2 in sodium chloride Ternary VLE (CO2-water-sodium chloride)
Ji et al. [492] Tan et al. [493]
Diamantonis and Economou [494] Rozmus et al. [495] Schreckenberg et al. [496] Sun and Dubessy [497]
Fig. 9. Status of original UNIFAC model group interaction parameter matrix using approach 3 for subgroup definition [506].
tural variations on the activity coefficient are not considered and a lot of parameters would be necessary to include an extensive list of cations [501]. Approach 2: This approach considers cation and anion skeletons as one entity [504]. It was credited by Lei et al. [501] for enabling the elimination of long-range electrostatic force term in activity coefficient calculation. However, if numerous cations and anions are to be considered, the parameter matrix would be very large. Approach 3: This approach separates each IL into a cation, an anion and their substituents (with imidazolium ion as a functional group) [505]. This approach is advantageous in the sense that it takes into account the impacts of structural variations of cation, anion and their substituents, and could result in the most compact parameter matrix. However, it would have highly extensive experimental data requirement for parameter regression. The existing IL-UNIFAC models extended for carbon dioxide solubility prediction (i.e. binary VLE) include original UNIFAC model and modified UNIFAC (Dortmund) model. For the original UNIFAC model, approach 2 was applied to regress interaction parameters for 22 ILs involving cations i.e. IM, PYR, PYRR, N and P ions, and
anions i.e. BF4, PF6, Tf2N, TfO, methylsulphate (MeSO4), ethylsulphate (EtSO4), chloride (Cl), diethylphosphate (DEPO4), dimethylphosphate (DMPO4), 2-(2-methoxyethoxy)ethylsulphate (MDEGSO4), NO3 and thiocyanate (SCN) ions [498]. In the associated modified UNIFAC (Dortmund) model, approach 3 was used but only involved ethyl (C2) - hexyl (C6) substituted methylimidazolium (MIM) cations and anions i.e. BF4, PF6 and Tf2N ions [482]. The group interaction parameter matrixes for original UNIFAC and modified UNIFAC (Dortmund) models applying approach 3 for subgroup definition are illustrated in Figs. 9 and 10, which are summarised based on the research outcomes of Hizaddin and Hadj-Kali [482], Kato and Gmehling [506], Nebig and Gmehling [507], Hector et al. [508], Paduszynski and Domanska [509], and Hector and Gmehling [510]. Despite being appealing in terms of compactness of interaction parameter matrix, they have not been extensively expanded for prediction of carbon dioxide solubility in ILs. More specifically, to date the modified UNIFAC (Dortmund) model developed by Hizaddin et al. [482] consists of five cations and three anions, and could only consider 15 possible IL combinations. In contrast, the ab initio
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Fig. 10. Status of modified UNIFAC (Dortmund) model group interaction parameter matrix using approach 3 for subgroup definition [482,506–510].
models have considered a more diverse array of ILs, as summarised in Table 13. Hence, UNIFAC model shall be extended to include these additional cationic and anionic species. Similarly, analogous UNIFAC model for prediction of ternary VLE phase equilibrium involving carbon dioxide, methane/hydrogen and ILs is still not existent. Specifically, relevant works included PR EOS model fitted by Ramdin et al. [511] for simulating ternary VLE of carbon dioxide/methane mixture with ILs, modified PR EOS developed by Shiflett et al. [512] and molecular simulation by Handy et al. [513] for separation of carbon dioxide from hydrogen sulphide via ILs, as well as soft SAFT EOS by Pereira et al. [514] and generic RK EOS by Shiflett et al. [515] for IL-based separation of carbon dioxide from nitrous oxide. It shall be noted that several important variants have been developed, and they are different from each other in terms of interaction parameter am;n formulations (with temperature as independent variable) and data type used for parameter regression. These UNIFAC variants are summarised in Table 14, whereby amn,0, amn,1, amn,2 denote regressed interaction parameters, T is temperature and T0 is room temperature.
7. Summary of research gaps In this section, potential research directions in the field of precombustion carbon capture and IL (as physical solvent) development are presented. For the former, research on the composite material or nanoparticle-based technology is required to optimise the stability of construction material against the corrosion issue and carbon fouling in the reformer section. In addition, future researchers
are also encouraged to find solutions for reducing the costs of carbon dioxide separation technologies, for instance by exploring the potential of more biomass materials, agricultural wastes and mine wastes for adsorbent (i.e. activated carbon and calcium oxide) synthesis. Functionalisation of MOF adsorbent material with multiple functional groups and metallic cations has also appeared as a new trend for improving the adsorption separation performance. In this particle field, focus shall also be put forward to the economics and availability assessment of the precious metals and raw ingredients. From the review of CAMD aspect, it has been identified that the current comprehensively developed IL-based UNIFAC models involve subgroup segmentation that results in bulky binary interaction parameter matrix, and therefore are inconvenient to use when cations and anions are to be chosen from comprehensive lists. Therefore, the UNIFAC model version considering cationic, anionic mainframe and substituent as separate subgroups (as in the work of Hizaddin et al. [482]) shall be further extended to include more IL constituents (i.e. phosphonium [P], ammonium [N], guanidinium [GUA] and morpholidinium [MOR]). To date, only original UNIFAC and modified UNIFAC (Dortmund) models have been extended for prediction of carbon dioxide solubility in ILs. KT-UNIFAC model, which has greater accuracy and could better describe the isomeric molecular difference of IL species, deserves further exploration for IL-based UNIFAC development. In addition, the current IL-based UNIFAC model should be extended to simultaneously simulate the VLE phase equilibrium of multiple gases (i.e. carbon dioxide/hydrogen and carbon dioxide/ methane) in a wider array of ILs for pre-combustion carbon capture solvent screening. This would be necessary for identification of functional groups sensitive to carbon dioxide/hydrogen and carbon dioxide/methane selectivities.
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Table 13 Coverage of ionic liquids in ab initio models. Solubility model
Description
Classes of ionic liquids (IL)
Ref.
COSMO-RS
12 cations and 6 anions; 72 ILs
Cation: imidazolium (IM), ammonium (N), phosphonium (P), and guanidinium (GUA); Anion: tetrafluoroborate (BF4), hexafluorophosphate (PF6), bis(trifluoromethylsulphonyl) imide (Tf2N), nitrate (NO3), triflate (TfO), and tris(pentafluoroethyl)trifluorophosphate (FEP) Cation: IM, PYR, PYRR, and sulphoniume (SUL); Anion: acetate, borate, phosphate/phosphinate, carbonate, salicylate, saccharinate, aluminate, acesulphamate, and cyanomethane Cation: IM, PYR, PYRR, N, P, quinolinium (Q), and isothiouronium (T); Anion: NO3, BF4, PF6, Tf2N, dicyanamide (DCA), thiocyanate (SCN), sulphonate, trifluoroacetate (TFA), and phosphate
Maiti [478]
212 cations and 63 anions; 13,356 ILs 170 ILs
Farahipour et al. [480] Palomar et al. [499]
COSMO-SAC
73 cations and 37 anions; 2701 ILs
Cation: IM, PYR, PYRR, N, P, GUA, PIP, souronium (U), T, Q, and aniline; Anion: acetate, borate, sulphonate, imide/amide, phosphate/phosphinate, and halogenide
Sumon and Henni [479]
Molecular simulation of hildebrand solubility parameters
21 cations and 10 anions; 210 ILs
Cation: IM, PYR, U, T, N, P, and GUA; Anion: acetate, sulphonate, Tf2N, TfO, phosphate, borate, PF6, and BF4
Sistla et al. [487]
8. Challenges of pre-combustion carbon capture technology 8.1. Commercial viability From global point of view, pre-combustion carbon capture technology has gained attention from the industrial players (especially coal and biomass gasification power plants) in the United States and European countries. However, this technology is still not widely commercialised worldwide since the enabling technologies (i.e. syngas-compatible industrial energy system, gas turbine system and fuel cell technology) are still largely at research stage. Therefore, the overall demand is far limited compared to postcombustion carbon capture technology. In Malaysia, hydrogen production technology (i.e. steam methane reforming and biomass gasification) is not practically existent despite having research progress to enable future application [529]. It shall be noted that most of the power plants in Malaysia being direct-fired type (either coal or biomass), which would be more compatible with post-combustion carbon capture system. Pre-combustion carbon capture system, on the other hand, is limited to new power plants since it has to be integrated from the conceptual design phase [45]. The local operating technological setting has inherently defied the need of pre-combustion carbon capture. Physical absorption using IL, on another part, poses another terrain of challenge for its commercialisation. In fact, despite having extensive modelling and simulation research works conducted on IL solvent design, IL has still not gained enough confidence level for commercialisation. 8.2. Financial constraint In terms of financial consideration, pre-combustion carbon capture system involves higher capital cost. For instance, capital expenditure of approximately USD 1169–1565/kW has to be invested for a single IGCC power plant with carbon capture, as reported by Thambimuthu et al. [44]. Furthermore, for existing power plants and other potential industrial sectors, its application would require a major retrofitting modification [45]. Moreover, the cost of ILs is prohibitively high for commercial usage, in contrast to the other conventional physical solvents, even if pre-combustion carbon capture is to be deployed.
At international scale, the existing driving forces i.e. IEA 2C limit and Kyoto treaties are all based on voluntary basis, and as such not seriously considered by the industrial and commercial players. In Malaysian scenario, there is no regulatory emissions limit for carbon dioxide, and carbon capture technology installation is not mandatory in contrary to the conventional air pollution abatement (for controlling the particulate matter, sulphur dioxide, carbon monoxide and nitrogen oxide emissions). According to Clean Development Mechanism (CDM) [530], termination of CDM programme at the end of 2012 had deprived all sustainability-related development projects of financial incentive through sales of certified emission reductions (CER) to the Europe’s Emissions Trading Scheme. This policy change would indirectly slow down the progress of CCS development among the local industrial players. 8.4. Technological constraint Despite already having several commercial-scale precombustion carbon capture facilities worldwide, there are still technical uncertainties in the operation and equipment design involved. For regions already implementing pre-combustion carbon capture, advanced technologies i.e. hydrogen turbine and acid gas shift conversion unit operation are highly complex, lacking reliability and vulnerable to unexpected accidents when upscaled to full commercial capacity [531]. Moreover, other technical problems comprise of fouling problem at reformer section (due to carbon deposition) and corrosion issue. Currently, research advancement for improving the operational efficiency, safety and health aspects of pre-combustion carbon capture technology is still in dire need. In Malaysia, obvious technical problem is the lack of professional technicians in Malaysia capable of monitoring the operation, troubleshooting and maintaining the CCS plant. Moreover, most of the advanced CCS technologies are still in laboratorial testing stage, and lack pilot, demonstration or full commercial-scale prototype for demonstrating their practical effectiveness. While reliance on the technology imported from foreign country would be prohibitively costly, slow research progress on CCS technology, lack of systematic analysis and updated technical information have made the research-to-commercialisation transition difficult.
8.3. Governance and regulatory framework 9. Future prospect of pre-combustion carbon capture Governmental incentives, long-term policies, CCS-based emission trading and regulatory framework, which are important to induce CCS investment, are lacking worldwide.
Despite the challenges above, pre-combustion system has high strategic significance due to flexible performance at large scale,
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 14 Summary of UNIFAC model variants. UNIFAC variant
Temperature dependency of parameter
Data for parameter estimation
Comment
Ref.
Original UNIFACVLE
Independent of temperature
Vapour-liquid equilibrium (VLE)
Recommended over narrow range of temperatures
Fredenslund et al. [516]; Fredenslund et al. [500]; Hansen et al. [502]
Original UNIFAC-LLE
Independent of temperature
Liquid-liquid equilibrium (LLE)
Limited application due to narrow temperature range around room temperature
Magnussen et al. [517]
Linear UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE
–
Hansen et al. [518]
Modified UNIFAC (Lyngby)
Logarithmic dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, Enthalpy of mixing (HE)
Modification on combinatorial term
Larsen et al. [519]
Independent of temperature
VLE, Activity coefficient of infinite dilution (c1), Water data
Suited for calculation of octanolwater partition coefficient
Chen et al. [520]
Quadratic dependence:
VLE, LLE
Suitable for water-hydrocarbon systems
Hooper et al. [521]
VLE, HE, c1
Modification on combinatorial term, and regression of r and q parameters
Wedlich and Gmehling [522]; Gmehling et al. [523]; Gmehling et al. [524]; Gmehling et al. [525]
þ amn;2 ðTlnðTT0 Þ þ T T 0 Þ Water-UNIFAC
Water-UNIFAC
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2 Modified UNIFAC (Dortmund)
Quadratic dependence:
KT-UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, HE, c1
Involvement of first-order and second-order estimations to overcome the problem of proximity effect and isomerism
Kang et al. [526]
KT-NIST UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, HE, c1
Involvement of first-order and second-order estimations to overcome the problem of proximity effect and isomerism; Involvement of higher-quality data compiled; Higher reliable, accurate and robust property prediction
Kang et al. [527]
UNIFAC-CI Modified UNIFAC-CI
Independent of temperature Quadratic dependence:
VLE, Solid-liquid equilibrium (SLE)
Regression of group interaction parameters not available in UNIFAC model
Mustaffa et al. [528]
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2
high thermal efficiencies, and capability to synthesise saleable products (i.e. electricity, hydrogen, fuels with lower carbon footprint, and chemical commodities) within reasonable carbon constraint. Decreasing availability of fossil fuel resources would induce gradual development and acceptance of various hydrogen production technologies (especially steam methane reforming technology) [529] and coal-based IGCC technology [532]. This indirectly creates the supply-demand chain to drive the commercialisation of pre-combustion carbon capture. Similarly, IL, although being economically infeasible and less competitive, would be a promising substituent (or solvent blend constituent) in the future for its low environmental impact and highly tuneable solvent properties. 10. Conclusion In conclusion, pre-combustion capture technology serves as one of the technically feasible alternatives for carbon capture in natural gas treatment, combined cycle gas turbine power plant, and coal gasification utilisation sector. Much ongoing research works are still in need to ensure the transition of this technology from research phase to full-scale commercial plants worldwide, provided sufficient funding from the government and relevant international non-governmental organisations (NGO). For the side of IL development as co-solvent for pre-combustion capture purpose, various experimental and simulation works have been conducted in local and international research institutes. In terms of CAMD
for IL solvent optimisation, IL-based UNIFAC model is a simple yet robust candidate to its more matures COSMO-based and SAFT counterparts. More work shall be conducted on development of novel pre-combustion carbon capture technologies, especially sorbent enhanced reaction and membrane reactor. For IL-based CAMD, more efficient subgroup decomposition method, inclusion of ternary VLE prediction capacity, extension of IL database, and development of second-order group-based UNIFAC model (i.e. KT-UNIFAC) shall be emphasised as future research scope. Acknowledgement Authors would like to acknowledge the funding support for this work provided by Ministry of Education, Malaysia and Universiti Teknologi Malaysia (UTM) under research grants Q. J130000.2501.10H28, Q.J130000.7809.4F618 and R.J1300000. 7301.4B145, as well as Japan International Cooperation Agency (JICA) under the scheme of Science and Technology Research Partnership for Sustainable Development (SATREPS) Program for the project Development of Low Carbon Scenario for Asian Region. References [1] IEA. Key world energy statistics; 2013. [2] IEA. World energy outlook 2010; 2010. [3] Matsuo Y, Yanagisawa A, Yamashita Y. A global energy outlook to 2035 with strategic considerations for Asia and Middle East energy supply and demand interdependencies. Energy Strat Rev 2013;2:79–91.
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Contents lists available at ScienceDirect
Applied Energy journal homepage: www.elsevier.com/locate/apenergy
Review of pre-combustion capture and ionic liquid in carbon capture and storage Wai Lip Theo a, Jeng Shiun Lim a,b,⇑, Haslenda Hashim a,b, Azizul Azri Mustaffa a,b, Wai Shin Ho a,b a b
Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia Process Systems Engineering Centre (PROSPECT), Research Institute for Sustainable Environment, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia
h i g h l i g h t s Important carbon capture technologies for pre-combustion capture. Review of physical solvents for pre-combustion capture with physical absorption. Review of solubility models for carbon capture. Challenges and future prospect of pre-combustion capture. Research gaps in ionic liquid-based UNIFAC model development.
a r t i c l e
i n f o
Article history: Received 20 July 2016 Received in revised form 5 September 2016 Accepted 26 September 2016
Keywords: Carbon capture and storage (CCS) Pre-combustion capture Ionic liquid (IL) UNIFAC model Computer-aided molecular design (CAMD) Review
a b s t r a c t Global warming issue, which increasingly aggravates over time, necessitates the carbon capture and storage (CCS) technology for its efficient mitigation. Among the major CCS technologies, post-combustion capture is the most established and commonly employed. However, it poses several energy and environment-related problems. As such, research and development of the pre-combustion carbon capture has been conducted to overcome the drawbacks of this conventional approach, and incorporation of ionic liquid (IL) has been increasingly given attention. This paper intends to review the carbon dioxide separation technologies and those related to IL in pre-combustion capture, pre-combustion capture research progress, pilot plant and commercial facilities, as well as modelling approach with special focus on the computer-aided molecular design (CAMD). In the last aspect, emphasis is given to the IL-based UNIFAC model, and key research gaps are identified from the review as general guidelines for the future research work and development in this particular field. Ó 2016 Elsevier Ltd. All rights reserved.
Contents 1. 2. 3.
4.
5.
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Introduction to pre-combustion carbon capture technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Important global research progress, pilot plants and commercial facilities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1. Pre-combustion capture research progress . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2. Pilot plant overview . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3. Commercial scale plant overview. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Carbon dioxide separation technologies for pre-combustion carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.1. Physical absorption technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.2. Adsorption technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.3. Membrane technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.4. Cryogenic separation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.5. Comparison of CO2 separation technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Ionic liquid in carbon capture and storage (CCS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
⇑ Corresponding author at: Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia (UTM), 81310 UTM Johor Bahru, Johor, Malaysia. E-mail address: [email protected] (J.S. Lim). http://dx.doi.org/10.1016/j.apenergy.2016.09.103 0306-2619/Ó 2016 Elsevier Ltd. All rights reserved.
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6.
Solvent design optimisation for pre-combustion carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6.1. Review of solubility models for carbon capture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6.2. Review of ionic liquid (IL)-based UNIFAC model. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7. Summary of research gaps. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8. Challenges of pre-combustion carbon capture technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.1. Commercial viability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.2. Financial constraint . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.3. Governance and regulatory framework . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8.4. Technological constraint . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9. Future prospect of pre-combustion carbon capture. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
1. Introduction Global warming has become more pronounced due to the immense carbon emissions from the fossil fuel-centred energy supply-demand chain worldwide. Currently, significant energy demand has continuously increased with increasing economic affluence of the modern society. According to International Energy Agency (IEA) [1], overall global primary energy demand in 2011 was already in the order of 550 exajoules. Moreover, it was anticipated to increase by 36% from 2008 to 2035 [2]. As a result, the global consumptions of petroleum, coal and natural gas were expected to increase at the annual rates of 1.2%, 1.4%, and 2.0% to reach the projected demands of 114 million barrels per day, 7000 million tonnes of coal equivalence, and 5000 billion cubic meters by 2035 [3]. This trend had led to carbon emissions up to 33.4 billion tonnes in 2011 [4]. According to Intergovernmental Panel on Climate Change (IPCC) [5], the global carbon dioxide concentration, without mitigation approach in place, would reach the range of 600–1550 ppm in 2030. Such transition in the atmospheric concentration of carbon dioxide has unequivocally led to warming of global climate system, leading to an increment in the global average temperature by 0.8 °C since 1880 [6]. If the problem were to be left to aggravate itself, the global mean surface temperature might increase by 2.5–7.8 °C by 2100, with consideration of climate uncertainties [7]. The global warming phenomenon would in turn exert negative impacts on the physical environment (i.e. increased global average temperature, sea level elevation, coastal region erosion [5], water cycle disruption, abnormal climate pattern, and ocean acidification [8]), biological ecosystem (i.e. endangerment of climate-sensitive and arctic species, wildfire destruction of fauna species, and occurrence of oceanic dead zones [8]), and human welfare (i.e. reduced water availability [9], food crisis [10], prevalence of water-borne diseases [11], and increased mortality associated with extreme weathers [5]). These crises, if left unresolved, could endanger the natural ecosystem and human civilisation. For effectively mitigating the global warming impacts, IPCC [7] indicated the need of keeping the global mean temperature elevation below 2 °C relative to the pre-industrial level. This would necessitate GHG emissions reduction by 40–70% as compared to 2010 level by 2050, and subsequently by 100% in 2100 [7]. Increased commitment has been seen through intensification of GHG emissions mitigation plans and strategies since 2012, whereby 67% reduction target of the global GHG emissions was officially enforced via regulations and policies [7]. The common policy instruments for GHG emissions reduction, especially for industrial and energy sectors, include voluntary approaches (VA), emissions trading, and emissions taxes [12]. Various adaptation and mitigation plans were recommended and evaluated by IPCC [7], and they encompass the following:
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i. Employment of low carbon intensive energy resources in place of coal, i.e. nuclear [13], natural gas [14], hydrogen fuel cell [15], and renewable energy resources (i.e. solar, wind, hydro, tidal, biomass and geothermal energy) [16]. ii. Enhancing energy efficiency of urban, industrial, and transportation sectors [17], and promoting energy conservation. iii. Geoengineering approaches, inclusive of carbon dioxide removal (CDR) and solar radiation management [18]. While there have been intensive researches devoted to exploring cleaner fuels and more efficient power generation technologies, the solutions however are still too expensive to be commercialised and widely applied. With more than 80% of overall energy demand currently being fulfilled by fossil fuel-based power plants, largescale emissions of carbon dioxide would be inevitable despite having these technological breakthroughs. Therefore, carbon sequestration via carbon capture and storage (CCS) approach is still the predominant strategy for global warming mitigation since it is technically and economically feasible with current cost range of USD 200–250 per tonne of carbon [19], has high carbon dioxide capture efficiency of more than 80%, and is compatible for intensive carbon dioxide point emission sources (i.e. power plants and heavy manufacturing industries) [20]. CCS is a large-scale separation of carbon dioxide from its significant sources followed by long-term isolation from the atmosphere and probably appropriate utilisation. It is an end-of-pipe solution tailor-made for the scenario whereby substantial emissions of carbon dioxide, associated with ever increasing global energy demand, industrial intensification and reliance on fossil fuel, are inevitable [21]. This approach is typically compatible for carbon sequestration from large-scale carbon dioxide point sources. The potential sectors for incorporation of CCS include power generation and heavy chemical manufacturing sectors.
Fig. 1. Global energy-related anthropogenic carbon dioxide emissions from 1990 to 2040 [22].
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As illustrated in Fig. 2, the energy-related anthropogenic carbon dioxide emissions had reached 32.27 billion tonnes by 2012. This figure is anticipated to elevate to 35.63 billion tonnes by 2020 and 43.22 billion tonne by 2040, whereby the majority of projected increase in carbon dioxide emissions is contributed by developing countries excluded from the Organisation for Economic Cooperation and Development (OECD) (as illustrated in Fig. 1) [22]. With all planned commercial CCS facilities worldwide, only 33.4 million tonnes of annual carbon capture capacity could be achieved by 2020, which is equivalent to 0.09% of the total estimated carbon emissions. For practical stabilisation of greenhouse effect, expansion of CCS technology would be in dire need.
In general, CCS technology could be categorised into postcombustion, pre-combustion and oxyfuel combustion capture types, as compared in Table 1. Fig. 2 illustrates the statistics of constructed commercial carbon capture facilities and capture capacity worldwide, and the details of the statistics shown are presented in Tables 2 and 3. It shall be noted that there is currently no operational full-scale CCS plant applying the oxyfuel combustion capture system. To date, post-combustion capture has been the most established CCS strategy with proven pilot projects and commercial scale plants. Solvent development and process intensification for post-combustion carbon capture using chemical absorption are
Table 1 Comparison of carbon capture technologies [23]. Aspect
Post-combustion capture
Pre-combustion capture
Oxyfuel combustion capture
Technology maturity level
Highly mature with numerous established applications at full-scale commercial plants
Well-established in process industries (typically water-gas shift reaction coupled with acid gas removal (AGR) process); Establishment of full-scale CCS plants under progress (mostly still in construction phase)
No full-scale oxyfuel-based CCS plants in operation; Limited to pilot-scale operations to date
Technical advantages
Highly compatible for retrofitting of existing power plants (enabling the continued use of common power generation technology i.e. pulverised coal); Comprehensive research in place to improve energy efficiency of postcombustion carbon capture equipment
Less energy-intensive carbon dioxide separation process (due to lower gas volume, higher pressure, and higher carbon dioxide concentration); More technologies commercially available for AGR process; Lower water consumption (as compared with post-combustion capture); Generation of hydrogen/synthesis gas as alternative fuel
Minimal emission of pollutants; No requirement of on-site chemical operations; Robust i.e. compatibility with a wide variety of coal fuels; Easier and simpler retrofit compared to post-combustion capture system; High carbon capture efficiency (on cost per tonne carbon dioxide sequestered basis) due to high carbon dioxide concentration; Reduced equipment size requirement; High maturity of air separation technology; High compatibility with conventional, high-efficient steam cycle without significant modifications; Highly established auxiliary equipment i.e. rotating equipment and heat exchanger
Technical disadvantages
Separation constraint imposed by low carbon dioxide partial pressure in flue gas; Commercially available amine scrubbing technology is often of small-scale and requires substantial upscaling; Significant energy penalty of amine scrubbing process (i.e. loss of 30% overall power output); Requirement of energy-intensive carbon dioxide compression; Most sorbent technologies are less robust with high performance requirement; Extensive water consumption
Significant energy loss due to sorbent regeneration (yet lower than that of post-combustion capture); Limited commercial availability of Integrated Gasification Combined Cycle (IGCC) technology; High auxiliary system requirement by IGCC technology; Syngas temperature swingassociated heat transfer problem; Reduced efficiency associated with hydrogen-fuelled gas turbine application
Infeasible development of sub-scale oxyfuel combustion capture technology; Net power output reduction due to energy-intensive air separation unit (ASU) and carbon dioxide compression; Technical uncertainties associated with operation of full-scale plant remain unresolved; Requirement of air-tight installation to avoid air leakage (or carbon dioxide leakage due to overpressurised operation); Possible corrosion problem
Economic aspect
High capital and operational expenditures due to large equipment size requirement (i.e. large flue gas volume)
IGCC capital cost is far higher than that of conventional coal power plant; High capital and operational expenditures for sorbent technology
High capital cost for air separation technology
Gas-fired: USD 1180 per kW Coal-fired: USD 1820 per kW
Gas-fired: USD 1530 per kW Coal-fired: USD 2210 per kW
Gas-fired: USD 0.097 per kW Coal-fired: USD 0.069 per kW
Gas-fired: USD 0.100 per kW Coal-fired: USD 0.078 per kW
Capital costa Gas-fired: USD 870 per kW Coal-fired: USD 1980 per kW Electricity costa Gas-fired: USD 0.080 per kW Coal-fired: USD 0.075 per kW a
Source: International Energy Agency Greenhouse Gas Programme [24].
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Fig. 2. Statistics of commercial carbon capture facilities worldwide.
well developed [42], and various solid sorbent technologies are continuously researched for its improvement [43]. However, it suffers several drawbacks, i.e. high regeneration enthalpy, thermal and oxidative degradation of amine-based solvents, and low carbon dioxide partial pressure constraint. Pre-combustion capture seems to be a promising alternative for overcoming these predicaments. As compared to extensive review by Thambimuthu et al. [44] and Kumar et al. [45], this review shall provide additional information about the current research programmes and advances in pre-combustion carbon capture development, pilot plant and commercial facility development status. Moreover, for modelling development of pre-combustion carbon capture optimisation, solubility model and particularly ionic liquid (IL)-based UNIFAC model are emphasised in this review. Challenges, future prospects and potential research directions are also provided. Following the introduction to pre-combustion capture technology in Section 2, important worldwide research progress, pilot plants and commercial facilities of pre-combustion carbon capture are presented in Section 3. Section 4 provides overview of carbon dioxide separation technologies for pre-combustion carbon capture. Moreover, reviews of ionic liquid in carbon capture and storage (CCS) and solubility model for carbon capture optimisation (with further emphasis on the IL-based UNIFAC model) are presented in Sections 5 and 6. This is followed by the summary of research gaps (Section 7), overview of challenges of pre-combustion carbon capture (Section 8), future prospects of pre-combustion carbon capture (Section 9) and conclusion (Section 10).
2. Introduction to pre-combustion carbon capture technology Pre-combustion carbon capture involves sequestration of carbon dioxide from fossil fuel or biomass fuel prior to completion of combustion process [46]. Its generic configuration is illustrated in Fig. 3. Typically, it is applied in (coal, natural gas and biomass) gasification and natural gas power plants [47]. A typical pre-combustion carbon capture system for gasification power plant, as depicted in Fig. 4, begins with gasification (or partial oxidation) of fuel to produce synthesis gas (or syngas) enriched with carbon monoxide and hydrogen. After particulate removal via cyclone separation unit, syngas is then processed in water gas shift (WGS) reformer wherein carbon monoxide reacts with steam to form carbon dioxide and hydrogen, and the resulted product stream is sent for desulphurisation and carbon dioxide separation
[44]. Ultimately, this carbon capture system generates hydrogen fuel stream for various power generation applications (i.e. gas boiler, gas turbine, fuel cell, etc.) with minimal sulphur dioxide generation, therefore raising the value of fuel by carbon content reduction [48]. Whereas in natural gas power plant, carbon dioxide separation unit is typically preceded by autothermal (steam) reforming and WGS processes [49]. Pre-combustion capture is often associated with process stream with higher carbon dioxide concentration (i.e. 15–60% by volume, dry basis), elevated pressure (i.e. 2–7 MPa) [51], and high temperature range of 200–400 °C [52]. Generally, the syngas stream after the catalysed WGS process has been reported to contain 64–73 mol % hydrogen and 20–23 mol% carbon dioxide [52]. High carbon dioxide partial pressure [48] in particular has thermodynamically driven the carbon dioxide adsorption with greater efficiency, and resulted in a lower energy demand for carbon capture and compression operation as compared to the post-combustion capture approach.
3. Important global research progress, pilot plants and commercial facilities 3.1. Pre-combustion capture research progress This section aims to review the research progress for precombustion carbon capture development worldwide. To date various research and development (R&D) works have been conducted to enhance the technological maturity and feasibility of precombustion capture technology. Significant research advances have been observed in the carbon separation technology development. Both simulation-based and experimental approaches were applied separately, or hand-inhand in these research works. Based on the literature research, adsorption, absorption, clathrate hydrate and membrane technology developments have been found to dominate the precombustion capture research domain. As shown in Fig. 5, adsorption technology has, inter alia, shown the most significant growth from 2009 to 2016. The references of reviewed literatures are presented in Table 4. Several transition trends have been noticed from the review. Firstly, for adsorption technology, the research focus evolves to novel/ modified materials (i.e. azo-linked polymer (ALP) [261], amine-modified titanium oxide [242], calcium oxide-based hollow sphere [250], melamine-modified phenol formaldehyde [257], mannitol-based ketal-linked porous organic polymer (MKPOP)
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 2 Summary of commercial post-combustion facilities worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Prosint Produtos Sintéticos, methanol production plant (Rio de Janeiro, Brazil)
Operating since 1967
90
Fluor’s Econamine FG Plus Process
Food-grade CO2 production
Rao et al. [25]
Kerr-McGee’s soda ash plant (Trona, California, USA)
Operating since 1978
800
Kerr-McGee/ABB Lummus Crest Process
Production of soda ash and liquid CO2
Barchas [26]
Lubbuck natural gas processing facility (Texas, USA) Indo Gulf Corporation Ltd, fertiliser plant (Jagdishpur, India)
1982–1984
1200
Fluor’s Econamine FG Plus Process
Operating since 1988
150
Enhanced oil recovery (EOR) application Urea production
Abu-Zahra et al. [27] Global CCS Institute [28]
300 MW coal-fired cogeneration plant (Poteau, Oklahoma, USA) Soda Ash Botswana soda ash facility
Operating since 1991
200
Food-grade CO2 production
Rao, Rubin [25]
Operating since 1991
300
Kerr-McGee/ABB Lummus Crest Process
Bellingham natural gas combined cycle power plant (Massachusetts, USA) Sumitomo Chemicals (Chiba, Japan) Liquid Air Australia (Two plants)
1991–2005
330
Fluor’s Econamine FG Plus Process
Operating since 1994 Operating since 1995
165 60
Production of food-grade CO2 for beverage production Food-grade CO2 production Food-grade CO2 production
Global CCS Institute [29] Rao, Rubin [25] Global CCS Institute [28]
Statoil’s Sleipner natural gas processing facility (Norway, North Sea)
Operating since 1996
2466
Amine scrubbing system
Oceanic storage at deep saline (Utsira) formation, 800–1000 meters below the sea bed
Global CCS Institute [30]
Petronas Fertiliser, steam reformer of fertiliser plant (Kedah, Malaysia)
Operating since 1999
160
MHI KM-CDR Process (using KS1 solvent)
Urea production
Iijima et al. [31]
Warrior Run 180 MWe coal-fired power plant (Cumberland, Maryland, USA)
Operating since 2000
330
Fluor’s Econamine FG Plus Process
Food processing, refrigeration and fire extinguisher production
Rao, Rubin [25]
Shady Point 320MWe coal-fired power plant (Oklahoma, USA)
Operating since 2001
800
Kerr-McGee/ABB Lummus Crest Process
Food and beverage processing, freezing and chilling purposes
Dooley et al. [32]
Chemical company, natural gas and oil-fired boiler (Kyushu, Japan) IFFCO/AONLA fertiliser plant (Aonla, India) IFFCO/PHULPUR fertiliser plant (Phulpur, India) Nagarjuna Fertilisers & Chemicals Ltd (Kakinada, India) Gulf Petrochemical Industries Company (GPIC) (Sitra, Bahrain) Ruwais Fertiliser Industries, natural gas reformer (Abu Dhabi, United Arab Emirate) Vietsovpetro White Tiger Project, Pyu-My 4000MW gas turbine combined cycle power plant (Pyu-My, Vietnam) Engro Chemical Pakistan Limited (ECPL), urea fertiliser plant (Pakistan)
Operating since 2005
330
General use product
Operating since 2006 Operating since 2009
450 450 450
MHI KM-CDR Process (using KS1 solvent)
Tatsumi et al. [33] Bandyopadhyay [34] Baron [35]
Operating since 2009
450
Urea and methanol production
Operating since 2009
400
Urea production
Operating since 2010
240
Operating since 2011
340
Enhanced oil recovery (EOR)/ enhanced gas recovery (EGR) application Urea production
National Fertiliser Ltd, Vijaipur plant (Madhya Pradesh, India)
Operating since 2012
450
Urea production
Qatar Fuel Additives Co. Ltd (QAFAC), methanol plant (Mesaieed, Qatar)
Operating since 2014
500
Methanol synthesis (yield enhancement)
Petra Nova Carbon Capture and Storage (CCS) Project, W. A. Parish coal-fired power plant (Texas, USA)
Under construction, operational by fourth quarter of 2016
4776
EOR at mature West Ranch Oil Field (Texas, USA)
Saskpower’s Boundary Dam Power Station (Saskatchewan, Canada)
Operating since 2014
2740
Cansolv Technology Inc. CO2 Capture Process
EOR at Weyburn Oil Field
MIT [40]
ROAD CCS Project, 1GW coal-fired power plant (Rotterdam, The Netherlands) Peterhead Project, 385 MW combined gas cycle turbine power plant (Scotland, United Kingdom) Bow City Power CCS Project, 1000 MW supercritical coal-fired power plant (Alberta, USA)
Under construction, operational by 2017 Under construction, operational by 2019
3014
N/A
Storage at depleted gas reservoir
MIT [41]
2740
Cansolv Technology Inc. CO2 Capture Process
Offshore storage at Goldeneye gas reservoir
Operational by third quarter of 2011
2740
Soda ash production
Production of urea, NPK, DAP, and NP Urea/ammonia production
Tatsumi, Yagi [33] Bandyopadhyay [34] Baron [35]
Mitsubishi Heavy Industries Ltd [36] Mitsubishi Heavy Industries Ltd [37] Mitsubishi Heavy Industries Ltd [38] Kamijo [39]
EOR
(continued on next page)
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Table 2 (continued) Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Shengli Oil Field EOR Project, Sinopec Qilu No.2 fertiliser plant (Shandong, China) Taweelah Project, natural gas-based TAPCO and EMAL power plants (Abu Dhabi, United Arab Emirates)
Operational by 2017
2740
N/A
EOR in Shandong Province
Operational by 2018
5479
N/A
EOR
Table 3 Summary of commercial pre-combustion facilities worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Pre-combustion capture plants Hydrogen Energy California Project, Hydrogen/petroleum coke-fuelled integrated gasification combined cycle (IGCC) power plant (California, USA) Texas Clean Energy Project, Coal-fired power plant (Texas, USA)
Constructed in 2015 and operational by 2020 Operational by 2019
8219
Onshore enhanced oil recovery (EOR) at Occidental’s Elk Hills Oil Field EOR at Bermian Basin
MIT [41]
Kemper County IGCC, Pre-combustion IGCC plant (Mississippi, USA)
Operational by 2016
9589
Rectisol AGR system Rectisol AGR system TRIGTM Technology
Killingholme Project, IGCC power plant (North Lincolnshire, United Kingdom) Don Valley Power Project, Coal-fuelled IGCC power plant (South Yolkshire, United Kingdom)
Operational by 2019
6849
Constructed in 2013 and operational by 2019 Constructed in 2013 and operational by 2015 Operational by 2020
13,425
Operational by 2015
Dongguan Project, Coal-fired 800 MW IGCC power plant (Dongguan, China) Huaneng GreenGen Project, Coal-fired 400 MW IGCC power plant (Bohai Rim, China) Lianyungang Project, Coal-fired 1200 MW IGCC power plant (Jiangsu, China)
5479– 8219
Onshore EOR
Selexol process Selexol process
Storage at deep saline formation
2740
TRIGTM Technology
EOR in Shandong Province
5479
N/A
EOR
2740
N/A
Oceanic storage at Binhai and EOR at North Jiangsu Oil Field
MIT [41]
Offshore storage at deep saline formation
Carbon Dioxide Storage Fuel
Carbon Dioxide Separation
Air
Exhaust Gas Fuel Combustion Heat & Power Fig. 3. Schematic diagram of pre-combustion carbon capture system [44].
[357], aramid [309], amine-modified molecularly imprinted polymer (MIP) [358], amine-impregnated silica nanotube [319], heterometallic MOF [318], multi-functionalised polymer [248], and multi-functionalised MOF [320]), composite materials (i.e. cadmium oxide/alkali metal halide mixture [135,179,244], hydrotalcite/graphene oxide composite [251], hydrotalcite/activated carbon composite [263], and metal oxyhydroxide/biochar composite [305]), and sustainable raw ingredients (i.e. mine waste [307], rice straw [247], and chitosan-based nano-composite [310]). Similarly, membrane-based research has also transitioned from single material exploration to composite membrane development [279,337,359], hybrid membrane contactor system [338,340], and mixed matrix membrane [283,339,341,342,360] for improved
performance. For clathrate hydrate separation process, different thermodynamic promoters (i.e. cyclopentane [58], tetra-n-butyl ammonium bromide (TBAB) [219], tetra-n-butyl ammonium chloride (TBAC) [295], tetra-n-butyl ammonium nitrate (TBANO3) [220], tetra-n-butyl ammonium fluoride (TBAF) [151], glucoamylase aqueous solution [347], and their mixtures [94]) and contact media (i.e. silica sand, water-saturated silica gel [74], cooled silica gel [158], glass bead [297], brine-saturated silica gel [196], metallic packing [291,294], alumina [223], coal bed [348,356], and waterin-oil emulsion [221]) have been tested. For absorption technology, the mainstream investigations have mainly dwelled in development and performance enhancement of solvents from 2011 to 2016, whereby the latest works have seen
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Syngas
CO2 Storage
CO2, H2
Fuel Steam Oxygen Cyclone Air Gasifier
Air Separation Unit (ASU)
Desulphurisation Column
CO2 Separator
Water Gas Shift (WGS) Nitrogen
Slag
Ash
Sulphur Exhaust Hydrogen Gas Turbine Air
Heat & Power
Fig. 4. Process flow diagram of pre-combustion carbon capture system for gasification power plant [50].
Table 4 References of reviewed pre-combustion capture research works.
Number of Published Research
45 40 35
Year
Carbon capture technology
Number of research
Refs.
30
2009
Adsorption Absorption Membrane Clathrate hydrate Hybrid
3 – 1 3 6
[53–55] – [56] [57–59] [60–65]
2010
Adsorption Absorption Membrane Clathrate hydrate Hybrid
5 – 2 4 1
[66–70] – [71,72] [73–76] [77]
2011
Adsorption Absorption Membrane Clathrate hydrate Hybrid
9 2 2 5 7
[78–86] [87,88] [89,90] [91–95] [96–103]
2012
Adsorption Absorption Membrane Clathrate hydrate Hybrid
11 2 6 6 4
[104–114] [50,115] [116–121] [122–127] [128–131]
2013
Adsorption Absorption Membrane Clathrate hydrate Hybrid
14 1 3 13 4
[132–145] [146] [147–149] [150–162] [163–166]
2014
Adsorption Absorption Membrane Clathrate hydrate Hybrid
42 2 6 9 15
[167–208] [209,210] [211–216] [196,217–224] [225–239]
2015
Adsorption Absorption Membrane Clathrate hydrate Hybrid
31 8 12 9 3
[240–270] [271–278] [279–290] [291–299] [300–302]
2016
Adsorption Absorption Membrane Clathrate hydrate Hybrid
27 5 8 10 6
[303–329] [330–334] [335–342] [46,343–351] [329,352–356]
Adsorption
25
Absorption
20
Membrane
15
Clathrate Hydrate
10
Hybrid
5 0 2009 2010 2011 2012 2013 2014 2015 2016
Year Fig. 5. Trend of pre-combustion capture research from 2009 to 2016.
the formulation of pure ionic liquid [331], hydrophobic physical solvent [332] and PEG-ionic liquid solvent blend [330]. Moreover, in recent years, with abundance of thermodynamics, kinetics, phase equilibria and cost databases, techno-economic and thermodynamic evaluations via simulations have gained popularity as pre-feasibility analyses prior to pilot and demonstration plant implementation [332,333]. It shall be noted that in contrast to other separation technologies lower number of published research in absorption is attributed to its transition to technology maturity phase, wherein the research communities are currently more engaged in implementing the pilot, demonstration and industrial-scale plants. 3.2. Pilot plant overview In tandem with the continuous research progress, many pilot testing programmes were carried out globally. Specifically, Vattenfall Group conducted a large-scale pre-combustion carbon capture validation programme prior to operation of commercial IGCC carbon capture plant in Buggenum, Netherlands. The purpose of this pilot testing is to obtain operational experience for coping with full-scale facility, verify the performance level of novel technology,
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and identify potential risks and mitigation measures. From the pilot testing, optimal system configuration, catalyst, solvent, construction material, upscaling strategy, and corrosion countermeasure were identified [361]. In Spain, ELCOGAS conducted pilot testing for examining the feasibility of pre-combustion carbon capture at Puertollano IGCC plant with hydrogen fuel synthesis, generating financial data for further upscaling purpose, increasing carbon dioxide recovery rate and reducing the carbon capture expenditure. The pilot plant research had demonstrated the technical and financial feasibility of upscaling the new technology to full scale (i.e. capacity of the existing gasification plant), and verified the operational robustness of pressure swing adsorption (PSA) technology [362]. Another successful pre-combustion carbon capture pilot study was implemented in the United States by Tampa Electric Company (TECO) in collaboration with the United States Department of Energy. In this pilot test, carbon dioxide solvency in amino acid salt formulation was examined while verifying the technical feasibility of novel technology anticipated to reduce the gasification plant operational cost [363]. Table 5 summarises the details of these pilot plant testing programmes. 3.3. Commercial scale plant overview In tandem with this research progress, many commercial scale pre-combustion carbon capture facilities have been built and operated worldwide. However, due to technological and financial constraints, physical absorption process still remains the most practical solution. Some of the commercial pre-combustion capture plants already in operational phase shall be discussed in detail as follows. Situated in Southwestern Kemper County, the Kemper County IGCC project consists of transport integrated gasification (TRIG) technology for fuel gas synthesis as feed to its combined cycle power generation system [364]. With TRIG technology, it could reportedly process 4.5 million tonnes per annum of low-quality lignite to produce synthesis gas sufficient for net power generation up to 524 MW [365]. The carbon capture facility of this project is based on physical absorption technology utilising Selexol process, which is able to reduce the carbon dioxide emissions by 67% with simultaneous synthesis of sulphuric acid (i.e. 135,000 tonnes per year) and ammonia (i.e. 20,000 tonnes per year) [366]. Another pre-combustion carbon capture facility that involves TRIG coal gasification process shall be featured by Dongguan Taiyangzhou IGCC power plant in Guangdong, China [367]. Being owned and operated by Dongguan Tian Ming Electric Power Co. Ltd. (TMEP), this 800 MW power generation facility is coupled with a cryogenic separation-based carbon capture facility with a capacity of 1 million tonnes per year. The captured carbon dioxide would be transported to off-shore gas/oil reservoirs for enhanced gas/oil recovery [41]. In Jiangsu, China, Lianyungang IGCC power plant
has also been constructed and operated by 2015 with a one-mil lion-tonne-per-year-capacity pre-combustion CCS system. Similarly, the captured carbon dioxide is transported via on-shore pipeline to the Northern Jiangsu oil-fields for enhanced oil recovery [41]. Table 6 shows the details of some commercial precombustion capture projects worldwide, all of which applying physical absorption technology. 4. Carbon dioxide separation technologies for pre-combustion carbon capture Typical carbon dioxide separation technologies for precombustion capture include physical absorption, adsorption, membrane, and cryogenic separation [20]. Each of these technologies is reviewed as follows. 4.1. Physical absorption technology Physical absorption technology includes two parts i.e. absorption and stripping processes, whereby in the former treated gas is contacted counter-currently with solvent stream and carbon dioxide is physically captured by the solvent whereas in the latter the carbon dioxide-saturated solvent is heated to regenerate the fresh solvent (to be recycled back to the absorption column) and release carbon dioxide at the top of stripping column (as illustrated in Fig. 6) [368]. Unlike the chemical solvents, extent of carbon dioxide absorption in the physical solvent is based on Henry’s law, i.e. linearly proportional to the partial pressure of carbon dioxide [370]. Without alteration of chemical identities of carbon dioxide and solvent [371], the dissolution of carbon dioxide in the liquid solvent is attributed to the van der Waals or electrostatic interaction between them, either of which being weaker than the chemical bonding as in the case of chemical absorption. Generally, physical absorption is optimal at high pressure and low temperature, while low pressure and high temperature conditions favour physical desorption [372]. With such pressure dependence of solvent loading, physical absorbent has better absorption performance than chemical absorbent at high partial pressure of carbon dioxide, while its regeneration could be easily achieved through depressurisation operation with lower energy demand (as compared to chemical absorption process) [44]. Therefore, it is more commonly used in precombustion carbon capture scenario, i.e. removal of carbon dioxide from synthesis gas as in IGCC power plants [361], natural gas treatment [48], as well as acid gas recovery (AGR) in coal or heavy oilfuelled chemical production processes (i.e. methanol, hydrogen, ammonia, substitute natural gas (SNG) and Fischer-Tropsch products) [370]. However, the absorption capacity of physical absorbent is only satisfactory at low temperature, therefore necessitating
Table 5 Details of pre-combustion carbon capture pilot plants worldwide. Pilot plant
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Puertollano, Coal and petroleum coke-fuelled integrated gasification combined cycle (IGCC) power plant (Puertollano, Spain)
Operational since 2010
100
Chemical absorption technology (using active methyl diethanol amine, aMDEA)
Recycled to IGCC process
Casero et al. [362]
Buggenum, coal and biomass-fuelled 253 MW IGCC power plant (Buggenum, The Netherlands)
Operational since 2011
34
Physical absorption technology (using dimethyl ether of polyethylene glycol)
Recycled to IGCC process
Damen et al. [361]
Polk Station, Coal-fuelled 250 MW IGCC power plant (Florida, USA)
Operational since 2014
822
Chemical absorption (Siemens POSTCAP Technology)
Storage at Lawson deep saline formation
Tampa Electric [363]
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 6 Summary of pre-combustion capture-based commercial-scale carbon capture plants worldwide. Commercial facility
Status
Capacity (TPD)
Capture technology
Final CO2 fate
Ref.
Hydrogen Energy California Project, Hydrogen/petroleum cokefuelled integrated gasification combined cycle (IGCC) power plant (California, USA) Texas Clean Energy Project, Coal-fuelled IGCC power plant (Texas, USA) Kemper County IGCC, Pre-combustion IGCC plant (Mississippi, USA)
Constructed in 2015 and operational by 2020 Operational by 2019
8219
Rectisol AGR systema
MIT [41]
Operational by 2016
5479– 8219 9589
Rectisol AGR system TRIGTM Technologyb; Selexol process
Onshore enhanced oil recovery (EOR) at Occidental’s Elk Hills Oil Field EOR at Bermian Basin
Nuon Magnum, Multi-fuel 1200 MW (coal, biomass and natural gas) power plant (Eemshaven, The Netherlands)
Operational by 2020
N/A
Selexol processc
Storage at North Sea Oil and Gas Fields
Damen et al. [361]
Killingholme Project, IGCC power plant (North Lincolnshire, United Kingdom) Don Valley Power Project, Coal-fuelled IGCC power plant (South Yolkshire, United Kingdom)
Operational by 2019
6849
Selexol process
MIT [41]
Constructed in 2013 and operational by 2019 Constructed in 2013 and operational by 2015 Operational by 2020
13,425
Selexol process
Storage at deep saline formation Offshore storage at deep saline formation
2740
TRIGTM Technology
EOR in Shandong Province
5479
N/A
EOR
Operational by 2015
2740
N/A
Oceanic storage at Binhai and EOR at North Jiangsu Oil Field
Dongguan Project, Coal-fired 800 MW IGCC power plant (Dongguan, China) Huaneng GreenGen Project, Coal-fuelled 400 MW IGCC power plant (Bohai Rim, China) Lianyungang Project, coal-fuelled 1200 MW IGCC power plant (Jiangsu, China)
Onshore EOR
a Rectisol AGR System is a patented pre-combustion carbon capture method developed by Linde and Lurgi. It is a cryogenic acid gas removal (AGR) process that applies methanol as solvent. b Transport Integrated Gasification (TRIGTM) technology is a cleaner and more economical coal-gasification method co-developed by Southern Company, KBR and Department of Environment (DOE) of the United States [41], due to its ability for efficient low-ranked coal utilisation. c Selexol process is a bulk carbon dioxide absorption technique that applies a mixture of dimethyl ether polyethylene glycols as solvent [361].
CO2 Clean Gas Condenser
Cooler
Absorber Column
Flue Gas
Lean Solvent
Stripper Column
Rich Solvent
Lean-Rich Solvent Heat Exchanger Reboiler
Pump
Pump Fig. 6. Simplified schematic diagram of absorption-stripping process [369].
the cooling of treated gas stream prior to absorption process and lowering the overall process energy efficiency [373]. The established commercial physical absorption processes include Selexol, Rectisol, Purisol [44], Morphysorb and Fluor processes [370]. While their solvent types and vendors are as summarised in Table 7, the advantages and disadvantages of these patented physical absorption processes are compared in Table 8.
Meanwhile, ILs comprise another class of novel physical solvents. They are a class of salts with melting points below room temperature and therefore exist in liquid phase at room temperature [383]. This is attributed to the weak coordination and ionic bonding between the ionic species, especially when bulky and asymmetrically configured organic cations are bonded with organic or inorganic anions [384].
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Table 7 Chemicals and vendors of different commercial physical absorption processes. Process Selexol process
c d e f
Dimethyl ether of polyethylene glycol (DMPEG) a
Purisol process
N-methyl-2-pyrolidone (NMP)a Morpholine
Operating conditions
Union Carbide (United States)
a
3.59 MPa and 35 °Cc
a
Methanol
Fluor process a
Vendor a
Rectisol Process
Morphysorb process
b
Chemical
3.6 MPa and 25°Cd
Lurgi and Linde (Germany) ; Lotepro Corporation (United States)a
b
Lurgi (Germany)a
15 to 0 °C and 6.8 MPae
Gas Technology Institute (GTI) (United States) b
Propylene carbonate
Fluor Daniel, Inc.
b
b
6.9 MPa and 48.8 °Cf 2.72–5.78 MPa and 25 °Ce
Thambimuthu et al. [44]. Jansen et al. [370]. Kapetaki et al. [374]. Sadegh-Vaziri et al. [375]. Spigarelli [376]. Gas Technology Institute [377].
Table 8 Advantages and disadvantages of different commercial physical absorption processes. Physical absorption process
Advantages
Disadvantages
Selexol process
High selectivity for H2S Does not require water wash for solvent recovery Chemically and thermally stable Low volatility (i.e. minimal solvent loss) Flexible i.e. compatible with combined removal of H2S and CO2, and specific H2S removal [370] Capable of moisture removal (due to hydrophilicity of solvent) Minimal capital and operational expenditures (i.e. carbon steel construction) [378]
High viscosity at low side of operational temperature (i.e. 0–175 °C), with reduced mass transfer rate and tray efficiency [275] Only suitable for CO2 removal if CO2 is more concentrated than H2S [378]
Rectisol process
Good CO2 and H2S removal efficiency (i.e. <0.1 ppm) to avoid catalyst poisoning (suitable for synthesis of methanol, hydrogen, ammonia, synthetic natural gas (SNG) and Fischer Tropsch products) Enable simultaneous capture of H2S and CO2 Reasonable viscosity of solvent Minimal solvent loss [370] Lower energy demand than amine-based absorption processes Minimal foaming and good miscibility with water High thermal and chemical stability Low corrosivity Minimal solvent degradation [378]
Low temperature operation (i.e. 30 to 80 °C) [379], requiring expensive and complicated cryogenic process stages Possibility of amalgam formation (due to absorption of mercury) at low temperature [378]
Purisol process
High selectivity for H2S Flexible i.e. compatible with combined removal of H2S and CO2, and specific H2S removal [370]
Volatile solvent and requirement of water scrubbing to avoid excessive solvent loss [370]
Morphysorb process
High solvent loading capacity Selective removal of H2S and CO2 Reduced corrosion Reduced environmental hazard Low capital and operating costs [380] Lower energy requirement [381] Lower recirculation requirement Lower co-absorption of hydrocarbon [382]
Relatively new process with low maturity level (i.e. at laboratory trial and pilot testing stages) [381]
Fluor process
Non-corrosive and low viscosity solvent Enable selective removal of H2S High solubility of carbon dioxide No requirement of make-up water [378]
Uneconomical to achieve high product purity Requirement of cryogenic operational condition Requirement of more efficient gas-liquid contactor [373] High solvent recirculation requirement Expensive solvent [378]
The potential of these novel solvents has been recognised due to their low volatility, non-flammable, and recyclable natures [385]. Apart from that, they are preferred over the conventional organic solvents for their enhanced solvation potential for a wide range of organic and inorganic solutes [386], high thermal stability [387], and wide liquid range [388]. Besides, their adjustable solvent (i.e. physiochemical) properties based on the choice of constituting cations and anions [384] endow them the designation of ‘designer solvents’. However, for (non-functionalised) physical ILs, carbon dioxide solubilisation mechanism could be attributed to the Lewis acid-
base interaction between carbon dioxide (i.e. Lewis acid) and anions (i.e. Lewis bases) [389], solvent free volume and van der Waals interaction [390]. In the first mechanism, cation adjustment has seen auxiliary effect on the improvement of the carbon dioxide solubility, and imidazolium-based ILs are the most widely investigated and applied ones. In particular, Almantariotis et al. [391] found that the carbon dioxide solubility would increase with larger alkyl group of imidazolium (IM) cation, and more significantly fluorination of cation. Despite the reported significant affinity of imidazolium cation-based ILs towards carbon dioxide, other cations i.e. choline (CHO) [392], ammonium (N) [393], pyrrolidium (PYRR)
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[394], pyridinium (PYR) [395], guanidinium (GUA) [396], piperidinium (PIP) [397] and phosphonium (P) [398] had also been investigated. Manipulation of IL anionic constituent would impose much more significant effect on its absorption capacity for carbon dioxide. In an experimental research by Aki et al. [399], carbon dioxide solubility was probed for different anions coupled with imidazolium cation, and it was found that the solubility increased in the order of nitrate (NO3) < dicyanamide (DCA) < tetrafluoroborate (BF4) < hexafluorophosphate (PF6) < triflate (TfO) < bis(trifluorome thylsulphonyl)imide (Tf2N) < methide anion. The increasing solubility trend is attributed to the increment in excess enthalpy of dissolution, which is primarily and secondarily contributed by the attractive van der Waals interaction and electrostatic bonding respectively. Despite their advantages over the conventional physical solvents, these ILs are still not ready for commercial-scale application due to its high viscosity and limited diffusivity, which could lead to unsatisfactory gas-liquid mass transfer (i.e. slow absorption rate) in the conventional absorption packed column [400]. Moreover, their prohibitively high costs have made it infeasible for absorption application in commercial-scale CCS facilities [401]. 4.2. Adsorption technology In contrast to the absorption process, adsorption involves selective formation of physical or chemical bonds between the carbon dioxide (adsorbate) and solid-phase adsorbent surface until the latter becomes saturated. Subsequently, adsorbed carbon dioxide is then desorbed through pressure swinging (as in pressureswing adsorption (PSA)) or temperature swinging (as in temperature-swing adsorption (TSA)) to regenerate the adsorbent material [44]. Typical sorbent technology configuration is similar to that of absorption process (Fig. 5). In TSA the saturated adsorbent is heated (using hot air or steam) to the temperature range at which the physical or chemical bond is broken to release the adsorbed species whereas in PSA pressure is reduced to achieve the same effect. It shall be noted that the former is preferred if the carbon dioxide concentration is not significant, while the latter is more compatible for the scenario whereby the carbon dioxide partial pressure is high [402]. In practical point of view, PSA is more appealing due to its shorter temporal requirement for adsorbent regeneration, and compatible with the economic need of bulk separation at full commercial scale (i.e. minimal idling time of adsorption bed) [44]. Theoretically adsorption has been reported to be superior in terms of high loading capacity at ambient conditions, less energy intensive and economical regeneration process, mechanical and chemical stability, high adsorption rate, simple operation and maintenance, and satisfactory tolerance with moisture and impurities in the flue gas [403]. Common physical adsorbents include activated carbon, zeolite [404], carbon molecular sieves, silica membrane and metal-organic framework materials (MOF) [405], whereas chemical adsorbents encompass calcium oxide (CaO), lithium metal-based sorbents and solid amine sorbents [404]. The technical details of these physical and chemical adsorbents are as summarised in Tables 9. 4.3. Membrane technology Membrane separation is a transport process based on Knudsen diffusion principle whereby the permeate (i.e. carbon dioxide) would dissolve in the membrane and diffuses through it at the rate proportional to its partial pressure gradient across the membrane [426]. According to Thambimuthu et al. [44], application of nonfacilitated membrane separation technology is more common to
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the carbon dioxide removal from natural gas (as in gas treatment process) and pre-combustion capture, whereby the carbon dioxide partial pressure is much higher. The proposed scheme of zero emission power plant utilising membrane technology is shown in Fig. 7. For the case of carbon capture from flue gas, since the carbon dioxide concentration is low, more energy penalty would be imposed (as compared to wet scrubbing process) due to requirement of compression work to ensure sufficient driving force for achieving the desired carbon capture ratio (CCR) and carbon dioxide purity [427]. Moreover, its selectivity could only be improved at cost of permeability, and vice versa [428]. Therefore, despite having advantages i.e. avoidance of steam utility, minimal environmental impact associated with solvent volatilisation and degradation, simple assimilation to the existing power plant [429], as well as design compactness and small footprint requirement [430], commercial application of membrane technology for postcombustion capture is still challenging. In view of such predicament, several alternative solutions have been introduced by the ongoing researches. One of the investigated alternative is facilitated transport membrane separation. It consists of mobile or fixed-site liquid phase carrier that enables active transport of carbon dioxide in the form of intermediate species i.e. bicarbonate. This would enhance the selectivity and permeability of carbon dioxide across the membrane [426]. Another class of modified membrane technology is constituted by mixed matrix membranes, which are polymer membranes impregnated with inorganic fillers [428]. The inorganic fillers tested include zeolite, carbon molecular sieve [431], MOF materials [430], zeolitic imidazolate framework (ZIF) materials [432], carbon nanotubes [433], titanosilicates and ordered mesoporous silica [434]. Such modification results in membrane with concurrent enhancement of selectivity and permeability, lower processing cost (due to polymer), better handing properties relative to inorganic membranes [428], good mechanical stability [431], better thermal stability and lower vulnerability to plasticisation (induced by high partial pressure of carbon dioxide) [435]. Gas membrane contactor (or hybrid membrane/solvent system) is another novel membrane-based separation technology gaining attention for development. In this system, separation is not based on Knudsen diffusion across the membrane but membrane only serves as a contacting medium between flue gas and carbon dioxide absorption solvent [426]. This modified technology exhibits the compactness of membrane system (and therefore lower capital cost), high selectivity (for carbon dioxide) of amine-based absorption process, and high flexibility for gas and liquid flow velocities [44], besides avoiding phase dispersion [426] and operational complications i.e. foaming and flooding [44]. The only disadvantage is the reduction of carbon dioxide mass transfer due to resistance imposed by the membrane framework [426]. 4.4. Cryogenic separation Cryogenic separation technology involves a series of cooling and compression operations at sub-ambient temperature and high pressure for separation of gaseous components in the carrier stream [436]. This technology has been widely used for production of high-purity liquid carbon dioxide (for food processing applications) and typically for pre-combustion captures process involving high carbon dioxide concentration (i.e. more than 90% by volume). Typical schematic diagram of cryogenic distillation unit is shown in Fig. 8. Cryogenic separation technology, in fact, overcomes some shortcomings of the conventional amine-based scrubbing process by avoiding excessive water consumption, need of expensive chemical agents, corrosion and foaming issues, need of winterisa-
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Table 9 Descriptions and comparisons of different physical adsorbents. Physical adsorbent
Description
Advantages
Disadvantages
Operating conditions
Activated carbon
Char material with high porosity, which could be activated physically or chemically; Physically activated carbon is formed via two (2)-stage process, i.e. pyrolysis of carbonaceous precursors at temperature below 800 °C to drive away volatile matters and form char, and activation of char with air/oxygen/steam/carbon dioxide; For chemical activation, precursors are first impregnated with dehydrating agent, followed by pyrolysis. Activation by chemical agent occurs simultaneously with charring process [403]
Suitable for low-temperature operation [404] High carbon dioxide capture capacity (of 10–15% by weight) due to highly porous structure/large adsorption surface area [404] Higher tolerance with water vapour [406] Inexpensive and low energy demand for regeneration [407] Long-term stability (i.e. negligible deactivation after 10 consecutive cycles) [407]
Lower selectivity for carbon dioxide over nitrogen than zeolite [407]
25 °C and 3 MPa [53]
Zeolite
Crystalline aluminosilicates with threedimensional framework enriched with cavities and channels through/in which small molecules, ions and entities may penetrate/ reside [408]
Suitable for low temperature operation [406] High loading capacity and selectivity for carbon dioxide [406] 5–10 times higher carbon dioxide/nitrogen selectivity than activated carbon [407]
Lower performance level when dealing with wet flue gas (because hydrophilic adsorption sites would be occupied) [406] Lower adsorption capacity [404]
0.72 MPa and 120– 200 °C [84]
Carbon molecular sieve
Special class of activated carbon with narrow pore distribution, engineered porosity, and capability of selective adsorption based on shape, size, adsorption rate difference, and discrepancy in adsorption equilibrium; Mainly made by controlled pyrolysis and carbon vapour deposition (CVD) techniques [405]
High tolerance with moisture content High resistance against corrosion by acids/alkalis High resistance against thermal degradation Higher selectivity for planar molecule (i.e. carbon dioxide) [405] Satisfactory permeability for carbon dioxide [409]
Costly and complicated manufacturing process (due to delicate nature of precursor material and risk of thermal expansion) [410]
5–35 °C and 0.1 MPa [411]
Mesoporous silica
Silica material with pore size between 2 and 50 mm, synthesised by reaction between soluble silica and surfactant template [412], organic template method in water/oil phase [413], and spray-drying of mixture of silica and polymer nanoparticles [414]
Large surface area for adsorption High capturing capacity (i.e. pore volume) Adjustable pore size High thermal and mechanical integrity [372] Low cost, harmless and chemically inert [413]
Not practical due to unsatisfactory carbon dioxide adsorption capacity at ambient pressure [372]
25 °C and 1– 3 MPa [415]
Metal-organic framework (MOF) material
Compounds assembled by metallic ions and organic ligands (containing nitrogen and oxygen elements), with one, two or threedimensional porous structure [416]
High surface area for adsorption Tunable pore structure and pore surface properties (via manipulation of metallic cation and ligand) High adsorption capacity at high pressure [372] High selectivity for carbon dioxide [416]
Performance level degradation due to presence of impurities (i.e. impractical) [372]
10 bar and 40 °C [417]
Calcium oxide (CaO)
CaO is used to chemically adsorb carbon dioxide in the form of calcium carbonate (CaCO3) at temperature greater than 600 °C in carbonation process; CaO could be regenerated via calcination at temperature above 900 °C [44]
High adsorption capacity High raw material availability Low cost of raw material [407] Established/long track record for industrial application Availability of high-level heat (from carbonation process) to be harnessed (i.e. for steam generation) and improve overall process energy efficiency [404] Durable and mechanically strong Fast adsorption/desorption rate [418]
Fast deactivation rate of calcium oxide and requirement of substantial replacement for practical operation [419]
650–950 °C, and 1– 42 bar [420]
Lithium-based adsorbent i.e. lithium silicate (Li4SiO4) and lithium zirconium (Li2ZrO3)
Chemical adsorption of carbon dioxide is elicited by the reversible reaction between lithium-based sorbent and carbon dioxide to form intermediates (i.e. for Li4SiO4, lithium carbonate (Li2CO3) and lithium metasilicate (Li2SiO3) [421]; for Li2ZrO3, Li2CO3 and zirconium oxide (ZrO2) [422] at temperature range of 500–700 °C; Adsorbent is regenerated by thermal decomposition of these intermediates
High capturing capacity Lower regeneration temperature compared to CaO (i.e. less than 750 °C) Sufficient adsorption/desorption rate High durability and stability (i.e. low performance decay rate) [421]
Low kinetics at high temperature (especially for Li4SiO4), requiring promoters to improve the performance [421] Expensive and difficult production due to scarcity and toxicity of raw materials [423]
400–600 °C and 1– 50 bar [424]
Amine-based sorbent
Solid support/nanoparticle/membrane with immobilised or impregnated amine solvent; The capture of carbon dioxide is based on the chemistry with amine
Low regeneration heat requirement (due to low heat capacity of solid sorbent) [372] High adsorption/desorption capacity Thermal stability at temperature up to 120 °C [404] Avoidance of corrosion problem High selectivity for carbon dioxide Proven tolerance with moisture content in flue gas [425]
Limited capture and regeneration efficiencies to make the process economically feasible [425] High cost [372]
25–85 °C and 0.1–1.0 CO2 partial pressure [241]
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Fig. 7. Proposed scheme of zero emission power plant utilising membrane carbon dioxide separation technology [44].
Fig. 8. Schematic diagram of cryogenic distillation unit [44].
tion modification [437], and pollution associated with emissions of solvent and degradation products [438]. This technology also offers the possibility of ambient pressure operation (i.e. avoiding associated hazards) and readily produces liquid carbon dioxide, therefore subsequently enabling economical carbon dioxide transportation [436]. Despite being one of the mature separation technologies, cryogenic separation process suffers several key problems. Firstly, due to operation at extremely low temperature (and high pressure), it
is very energy intensive (i.e. approximately 6–10 MJ per kg of recovered carbon dioxide) and therefore involves significantly high operational expenditure [20]. Moreover, possibility of ice formation in cryogenic process may lead to blockage of piping system and significant pressure drop, leading to possible equipment safety problem [439]. This necessitates the removal of moisture content prior to separation and therefore more financial investment on the required dehydration pre-treatment. In addition, frost (i.e. water and carbon dioxide) formed during operation may
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Table 10 Multi-faceted comparison of carbon dioxide separation technologies. Aspect
Physical absorption
Adsorption
Membrane technology
Cryogenic separation
Ref.
Technical advantages
Most established for precombustion carbon capture; Recoverable physical solvent from regeneration
Reversible process and recoverable adsorbent; High adsorption efficiency (of more than 85%)
Mature technology; Long track record for industrial carbon dioxide recovery
Leung et al. [20]
Technical disadvantages
Significant heat requirement for solvent regeneration; Absorption efficiency depends on carbon dioxide concentration; Possible environmental impacts from solvent degradation
Requirement of high temperature adsorbent; High energy requirement for carbon dioxide desorption
High commercial availability; High separation efficiency (of more than 80%) Operational issues i.e. low fluxes and fouling
Carbon dioxide separation yield (%) Energy Requirement (MJ/kg CO2)
90–98
80–95
80–90
>95
4.0–6.0
2.0–3.0
0.5–6.0
6.0–10.0
accumulate around the heat exchanger, increasing undesirable insulation and decreasing the heat transfer efficiency [436]. 4.5. Comparison of CO2 separation technology The technical advantages and disadvantages, carbon dioxide separation yield, energy requirement, environmental impact and financial aspect of the carbon dioxide separation technologies discussed above are summarised in Table 10. 5. Ionic liquid in carbon capture and storage (CCS) As mentioned in Section 3, physical absorption remains the most practical solution among the carbon dioxide separation technologies. Apart from the existing conventional physical solvents, the research community is still in a frenzy venture of discovering new pure solvents and solvent blend formulations with better properties. Among these experimental trials, ILs have stood out as a popular agenda due to their tunable solvent characteristics, thermal stability, minimum volatile loss, and reduced degradation-related emissions. This section reviews the IL-based carbon capture research and development. Main research scopes for IL-based carbon capture application comprise of biogas/natural gas upgrading as well as carbon capture at heat and power generation sites. For each scope, IL-based carbon separation technology development, optimisation, and techno-economic analysis for potential commercial facilities have been conducted. Specifically, for absorption-based biogas upgrading process, García-Gutiérrez et al. [440] had conducted techno-economical assessment on physical absorption-based biogas upgrading process using 1-ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [emim][Tf2N], 1-hexyl-3methylimidazolium bis[(trifluoromethyl)sulfonyl]imide [hmim] [Tf2N] and trihexyl(tetradecyl)phosphonium bis[(trifluoromethyl) sulfonyl]imide [thtdp][Tf2N], and found that the costs of these facilities were in the range of USD 9.18-11.32/GJ (lower heating value) with overall efficiency of 71–86%. In another study concerning the optimisation of thermodynamics and mass transfer properties of IL-polyethylene glycol dimethyl ether (NHD) mixture for biogas upgrading purpose, Zhang et al. [441] found that the optimum composition with maximum carbon dioxide/ methane selectivity was 50 wt% IL and 50 wt% NHD. In a solvent screening investigation, Privalova [442] assessed the solvent performances of aqueous amine solutions, conven-
Only viable for high carbon dioxide concentration (i.e. more than 90% by volume); Sub-zero temperature requirement; Significant energy penalty
Mondal et al. [436]
tional ionic liquids, ‘switchable’ ionic liquids and poly(ionic liquid)s, and found 1-butyl-3-methylimidazolium acetate [bmim] [Ac] the most promising with high carbon capture efficiency and 65 wt% VOC elimination. Moreover, Xie et al. [443] had evaluated the energy performances of biogas upgrading processes using [bmim][Tf2N], [hmim][Tf2N] and 1-butyl-3-methylimidazolium hexafluorophosphate [bmim][PF6] via simulation studies, and found that [bmim][Tf2N] was associated with the lowest energy intensity with energy consumption 11% lower than the water scrubbing process. For novel IL-based separation technology development for biogas/ methane upgrading purpose, Hojniak [444] assessed the selectivity of supported IL membrane (SILM), and indicated that tri(ethylene glycol) and nitrile groupfunctionalised imidazolium and pyrrolidinium ILs had 2.3 times greater carbon dioxide/methane selectivity compared to those functionalised with glycol group only. Whereas Wang et al. [445] had developed an IL-tethered activated carbon granule for packed bed adsorption with adsorption capacity of 2.95 mmol/g, carbon dioxide/methane selectivity of 95% and high multi-cyclic stability at the optimal conditions of 0.5 MPa and 20 °C. In another study, Singh, Cowan [360] optimised the performance of poly(ionic liquid)-ionic liquid-zeolite mixed matrix membrane by manipulating zeolite particle type, zeolite particle loading, poly(ionic liquid) structure, quantity of crosslinking, and zeolite dispersion pattern. Similarly, Nayak [446] developed IL-immobilised Matrimid mixed matrix membrane to overcome instability of the conventional SILM in high pressure application, and found that incorporation of MOF i.e. Cu3(BTC)2 would increase its carbon dioxide and methane permeabilities to 240 and 843 barrer. Besides, Cheng et al. [447] evaluated the adsorption performance of molecular sieve impregnated with phosphonium-based IL for upgrading of biogas into vehicle fuel, wherein IL-loaded molecular sieve was found to exhibit greater carbon dioxide adsorption rates compared to the pure analogous IL in both pure carbon dioxide and biohythane atmospheres. For power plant carbon capture purpose, Gao et al. [273] had developed an IL-tailored amine aqueous solution comprising of 30 wt% N-methyldiethanolamine (MDEA), 3 wt% piperazine (PZ), 57 wt% water and 10 wt% butyl-3-methylimidazolium tetrafluoroborate [bmim][BF4] with reduced sensible heat, highest carbon dioxide solvency potential and lowest solvent regeneration enthalpy. In addition, Luo et al. [448] introduced a modified amino-functionalised IL with incorporation of N or O atom for carbon capture; this new solvent had reduced viscosity, greater mass transfer, and reduced column size requirement due to the
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formation of intra-molecular hydrogen bonding. Hydrophobic IL solvent i.e. allyl-pyridinium bis(trifluoromethylsulfonyl)imide was also synthesised by Siefert, Agarwal [332] for precombustion capture at IGCC plant with lower levelised cost of carbon capture (LCOC) compared to Selexol process. Apart from solvent development for absorption process, Otani et al. [449] had developed facilitated transport membrane (FTM) loaded with triethyl(methoxymethyl)phosphonium pyrrolide, which was found to have maximum reactivity with carbon dioxide and superior rheological property. While Li et al. [450] had developed stronger [bmim][Tf2N]-ZIF-8 filler material for the synthesis of mixed matrix membrane with enhanced tensile strength, carbon dioxide flux and selectivity, Ma et al. [451] incorporated aminebased task specific IL (TSIL) into MOF (i.e. NH2-MIL-101(Cr) to synthesise highly carbon dioxide selective mixed matrix membrane with improved carbon dioxide permeability (i.e. 2979 barrer). In a study for evaluating the potential of amino acid IL (AAIL) as carbon dioxide carrier in FTM, Kasahara et al. [452] found that AAIL with greater amino acid density increased the FTM carbon dioxide permeability and selectivity. Whereas Deng et al. [359] synthesised a composite membrane with incorporation of cellulose acetate (CA) and ether-functionalised pyridinium-based IL, with significant improvement in carbon dioxide permeability. In addition, Tengteng et al. [453] had synthesised SILM from PEG-200 and choline prolinate [Cho][Pro] for toxicity reduction and cost effectiveness enhancement. In terms of the development of supported ionic liquid phase (SILP), Pohako-Esko et al. [454] found that IL-modified chitosan ionogel (formed by dissolution of chitosan in IL) encapsulated with nanoporous fumed silica had exhibited improved carbon dioxide adsorption capacity while Gouveia et al. [455], from the assessment of the potential of cyano and amino acid-based IL mixtures for SILP synthesis, indicated that ILs with L-alanine and taurinate anions were associated with high carbon dioxide permeability and selectivity. Moreover, Styring et al. [456] had screened the optimal solid IL (SoIL) for pressure swing adsorption application via molecular simulation approach. In another study; in this analysis, SoIL was found to have high adsorption selectivity, moderate adsorption capacity, fast adsorption kinetics, low volatile loss and great thermal stability. Besides, Mahmood et al. [457] synthesised an IL polymer from 1-vinyl-3-ethylimidazolium bromide and 1-vinyl-3ethylimidazolium bis (trifluoromethyl-sulfonyl) imide, with incorporation of activated carbon; the resulted polymers had greater carbon dioxide adsorption capabilities due to combined actions of absorption and adsorption. Apart from that, Zhou et al. [458] had developed alpha zirconium phosphate (ZrP) and montmorillonite (MMT) hybrid inorganic nano-sheets incorporated with 1butyl-3-methylimidazolium chloride, which exhibited carbon adsorption capacities of 0.73 mmol/g and 0.42 mmol/g at the optimum operating temperatures of 60 and 70 °C. For more efficient carbon capture at power generation facility, Lu et al. [459] had developed a hybrid carbon capture technique coupling the membrane contactor and membrane vacuum regeneration. In this study, aqueous [bmim][BF4] and 1-(3-aminopropyl)-3-methyl-imi dazolium tetrafluoroborate [apmim][BF4] solutions were associated with the optimal water contents of 60 mol% and 40 mol%, and the latter was found to have greater carbon dioxide loading capacity while the former exhibited higher regenerability (at low vacuum degree). In a similar fashion, Dai et al. [338] evaluated the materials for the synthesis of porous and non-porous hollow fibre membranes loaded with 1-butyl-3-methylimidazolium tricyanomethanide, and selected porous PTFE membrane and nonporous Teflon-PP composite membrane for membrane reactor development. Both materials had comparable mass transfer performance, while the latter exhibited greater stability during operation.
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Apart from the carbon dioxide separation technology development, Valencia-Marquez et al. [460] had conducted a technoeconomic and dynamic analyses on an IL-based carbon capture pilot plant, and indicated that it had lower energy demand and could tolerate with fuel gas flow rate fluctuation by 10% with satisfaction of specified carbon dioxide recovery and purity requirements. Moreover, from the controllability analysis conducted on an IL-based pilot-scale carbon capture plant, Valencia-Marquez et al. [461] had developed and optimised an efficient and decentralised multi-loop control system for enhancing its economics, safety level, operational robustness and environmental sustainability.
6. Solvent design optimisation for pre-combustion carbon capture To date, many carbon capture plants based on pre-combustion capture configurations have been planned, constructed and prepared for steady-state operation. In the future, these carbon capture technologies would become even more important in order to mitigate the global warming effect (i.e. to achieve desirable 2C Scenario), provided the ever increasing carbon dioxide emissions from power generation and heavy industrial sectors. Physical absorption technology still remains dominant in the pre-combustion carbon capture sector, with established track records as well as numerous patented processes being commercialised worldwide [462]. As part of the carbon capture process optimisation, many ongoing researches have been directed to optimisation of solvent design, with the aim of formulating new solvents and solvent blends with optimal characteristics. For carbon capture purpose, these selection criteria encompass better absorption capacity and selectivity, easy desorption (i.e. lower regeneration heat requirement), higher thermal and chemical stabilities, greater resistance against oxidative degradation, lower volatility and solvent loss, and lower toxicity and environmental impacts [463]. Conventional solvent design approach is basically bottom-up, i.e. combination of physicochemical knowledge base, expert judgment and experience, and empirical trials (i.e. laboratory synthesis of solvent formulation and testing) [464]. These approaches first identify molecules from the raw materials, and then scrutinise the preferred properties from the identified molecules [465]. Since these approaches identify compatible solvent candidates via trialand-error manner, they are generally time-consuming, expensive, tedious and posing certain hazards to experimenters despite guaranteeing the accuracy and reliability of results. Screening of solvent through property database is another simple approach, but its effectiveness relies on the extensiveness and accuracy of existing database. Moreover, it is not time and cost-effective [466]. Computational thermodynamics is a more appealing approach. Known as computer aided molecular design (CAMD), it is defined as a reversed engineering approach that generates feasible molecules from the specified building blocks which meet the targeted chemical properties. In some way, this approach first translates the desirable chemical product attributes into measurable physical properties, and then design molecular structures with the identified properties under specified constraints [467]. CAMD is a more systematic and efficient way of designing promising candidate solvents from the existing fundamental building blocks and database, therefore narrowing the scope of combinatorial experimental solvent screening down to a few promising ones only as well as achieving significant saving in terms of time and cost. According to Gani [467], CAMD design framework consists of four main steps, namely problem formulation (i.e. specification of desirable solvent properties), initial search (i.e. preliminary
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identification of functional group/molecule compatible with identified pure component properties from the existing property database), generation of molecular structures (using appropriate CAMD techniques) and evaluation of their properties (benchmarked against desired ones specified in the first step), and verification (i.e. simulation of chemical process using the designed candidate). Therefore, property prediction models are very essential tools in CAMD, and the reliability of CAMD-based solvent design outcome largely depends on their accuracy and robustness. Among them, solubility model that accurately predicts the phase equilibrium of all components in the carbon capture system (i.e. gas stream and solvent stream) is of utmost importance, since it is related to other essential solvent attributes i.e. solvent loss, selectivity and solute distribution coefficient [466]. Therefore, there have been ongoing research and development works for improving the solubility model of carbon dioxide in various solvents and solvent blends. 6.1. Review of solubility models for carbon capture To date, numerous models have been developed for prediction of carbon dioxide solubility in various physical and chemical solvents, as well as solvent blends. For phase equilibrium modelling, both homogenous and heterogenous approaches are possible, whereby for the former equation of state (EOS) models are commonly applied whereas for the latter chemical potentials of gas and liquid phases are separately computed. While gas-phase chemical potential (i.e. fugacity coefficient) is usually calculated using EOS models, liquid-phase chemical potential (i.e. activity coefficient) evaluation models comprise of ab initio (first principle), semi-empirical and empirical models, as listed in Table 11. Their brief technical details are as summarised in Table 12. From the summary, it could be seen that recent development has been focusing on the prediction of carbon dioxide solubility in ILs due to its advantages over the conventional amine-based solvent formulations. The developed solubility models include quantum mechanics-based models (i.e. Conductor-like Screening Model
Table 11 Categorisation of models applied for prediction of carbon dioxide solubility in different solvents. Ab-initio model
Semi-empirical model
Empirical model
Conductor-like Screening Model for Real Solvents (COSMO-RS) Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC)
Modified UNIFAC (Dortmund)
Molecular dynamics simulation of Hildebrand’s solubility parameter
Electrolyte NRTL (E-NRTL) model
Modified Kent Eisenberg (MKE) model Quantitative structure-property relationship (QSPR) model Artificial neural network (ANN)
Non-random Twoliquid (NRTL) model
Debye-Huckel (DH) model Extended DebyeHuckel (EDH) model Pitzer model
Statistical Associating Fluid Theory (SAFT) variants Group Contribution (GC) Equation of State (EOS)
Multilayer perceptron network (MLP) Least square support vector machine (LSSVM) Adaptive neuro inference system (ANFIS) Committee machine intelligent system (CMIS)
for Real Solvents (COSMO-RS), Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC) and molecular dynamics simulation), semi-empirical models (i.e. modified UNIFAC (Dortmund) model, Group Contribution Equation of State (GC EOS), Perturbed Chain Hard Sphere (PCHS) model, and Soft Statistical Associating Fluid Theory (Soft-SAFT) model), and empirical model (i.e. Quantitative Structure-Property Relationship (QSPR) model). While COSMO-based models and statistical molecular models (i.e. SAFT EOS variants, GC EOS, lattice models, etc.) have been extensively developed for systematic screening of ILs for carbon capture purposes, limited work had been conducted in exploring the capability of UNIFAC model variants in prediction of carbon dioxide solubility in ILs. In particular, only UNIFAC model [498] and modified UNIFAC (Dortmund) model [482] were regressed for predicting solubility of carbon dioxide in ILs. Moreover, in these works, the IL-based solubility databases applied were much less extensive compared to those in COSMO-based model development, and only binary vapour-liquid equilibria (VLE) was investigated. COSMO-based models, despite requiring minimal experimental data due to its predominant dependence on quantum mechanical information of chemical species, were found to erroneously predict the carbon dioxide solubility trend [499]. Moreover, the optimisation of structural configuration of molecules/ionic systems (based on minimisation of potential energy) as well as quantum mechanical computation of surface charge density (in the form of sigma profile) is computationally extensive and complicated. Another much developed counterpart i.e. SAFT models involve complex formulations with numerous pure component parameters and cross-association binary parameters, and therefore limit its applications in engineering field [498]. On the other hand, group contribution model is simpler to apply and has received increasing attention due to its increasing assimilation in many commercial process design simulation software (i.e. Aspen Plus, Aspen Hysis, PROII, Chemcad, ROMeo and Dynsim). More detailed review of IL-based UNIFAC model is as presented in Section 3.2. 6.2. Review of ionic liquid (IL)-based UNIFAC model UNIFAC group contribution model is designed to predict the liquid-phase activity coefficient in non-ideal liquid mixture [500]. In any variant of the UNIFAC model, the activity coefficient of a compound in multi-component mixture is considered as the summation of all functional group activity coefficients, each arising from interaction of any two specific functional groups. These interactions result in combinatorial and residual group contributions to the overall molecular activity coefficients, whereby the former is attributed to the disparity in the molecular shapes and sizes of interacting structural groups and the latter by disparity in their molecular interaction types [501]. The combinatorial group contributions of functional groups to the activity coefficient was derived based on the Staverman potential as in UNIQUAC model [500], and involve group surface area (Q k ) and volume (Rk ) parameters. Whereas the residual group contributions, computed using the UNIQUAC residual term calculation method [500], are related to the group area fraction and parameter associated with group energetic interactions (wmn ). The group surface area, volume and interaction parameters for a massive number of structural groups were comprehensively reviewed and revised for improvement [502]. For UNIFAC models extended for IL solvent screening, there are three approaches for establishing the subgroups of ILs, as described as follows: Approach 1: This approach considers separation of each IL into a cation and an anion [503]. Since the substituents on each cationic species are not separated as subgroups, the impacts of their struc-
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 12 Summary of solubility models for prediction of carbon dioxide solubility in different solvents. Solvent type
Model (chemical potential calculation)
System type
Ref.
Binary vapour-liquid equilibrium (VLE) (C1 - C5 alcohols)
Hsieh et al. [468]
Gas-phase
Solvent-phase
Alcohols
Peng-Robinson-Stryjek-Vera (PRSV) equation of state (EOS)
Conductor-like Screening Model for Segment Activity Coefficient (COSMO-SAC)
Alkanes
Homogenous approach Statistical Associating Fluid Theory for Potentials of Variable Range (SAFT-VR)
Ternary VLE (CO2 - methane - octane system)
Keskes et al. [469]
Amines
Soave-Redlich-Kwong (SRK) EOS
Quaternary VLE (mixture of three amines) Binary and ternary VLE (monoethanolamine (MEA), diethanolamine (DEA) and 2-amino-2methyl-1-propanol (AMP)) Binary VLE (MEA, DEA, AMP, methyl diethanolamine (MDEA), triisopropanolamine (TIPA) and 2amino-2-ethyl-1,3-propanediol (AEPD) ⁄ Include ionic species resulted from degradation of MEA; Ternary and quaternary VLE
Haghtalab and Ghahremani [470] Park et al. [471]
N/A
Peng Robinson (PR) EOS
Second-order virial equation
Electrolyte Non-random Twoliquid model (E-NRTL) Modified Kent-Eisenberg (M-KE) model
M-KE model; Extended Debye-Huckel (E-DH) model; Pitzer model NRTL model for molecular species; Debye-Huckel model for ionic species
Homogenous approach Electrolyte SAFT-HR (eSAFT-HR) Alternative Feed-forward multi-layer neural network model Alternative Multilayer perceptron network (MLP); Genetic algorithm - radial basis function network (GA-RBF); Coupled simulated annealing - least square support vector machine (CSA-LSSVM); Adaptive neuro inference system (ANFIS); Particle swarm optimisation - ANFIS (PSO-ANFIS); Committee machine intelligent system (CMIS)
Ternary VLE (Aqueous MDEA solution) Ternary/Quaternary/Higher VLE Quaternary VLE (aqueous mixture of MDEA and N-methylpyrrolidone (NMP))
Goharrokhi et al. [472]
Ostonen et al. [473]
Najafloo et al. [474] Hamzehie et al. [475] Tatar et al. [476]
Ester mixtures
Ideal gas assumption
Empirical EOS based on Hildebrand’s solubility parameter
Ternary VLE
Gui et al. [477]
Ionic liquids (IL)
SRK EOS
Conductor-like Screening Model for Real Solvents (COSMO-RS) COSMO-RS model
Binary VLE
Maiti [478]
Binary VLE; Estimation of Henry’s constants of CO2, nitrogen and methane in 2701 ILs Binary VLE; Estimation of Henry’s constants of CO2 in 13,356 ILs Binary VLE; Consider selectivity of CO2 over nitrogen, methane and hydrogen Binary VLE
Sumon and Henni [479]
Not relevant (i.e. Henry’s constant estimation)
Ideal gas assumption
COSMO-SAC model
Predictive SRK (PSRK) EOS
Modified UNIFAC (Dortmund)
Homogenous approach Perturbed Hard Sphere Chain (PHSC) EOS Homogenous approach Soft-SAFT Homogenous approach Group Contribution (GC) EOS Alternative Quantitative Structure-Property Relationship (QSPR) Alternative Molecular simulation of Hildebrand solubility parameters Polymers
Alternative QSPR
Electrolyte solutions/water
PRSV EOS
Electrolyte variant of UNIQUAC model
Homogenous approach Modified ion-based SAFT (SAFT2-KMSA) EOS Homogenous approach
Binary VLE Binary VLE (of CO2 and N2O in various ILs) Prediction of solubilities of CO2, CO, hydrogen, methane and ethane in [Cnmim][Tf2N] family ILs Binary VLE
Farahipour et al. [480] Lee and Lin [481]
Hizaddin et al. [482] Bazargani and Sabzi [483] Pereira et al. [484] Pereda et al. [485]
Eike et al. [486]
⁄Solubility parameters of CO2, methane, nitrogen, hydrogen, sulphur dioxide and nitrogen oxides in ILs
Sistla et al. [487]
Binary SVE (Polyethylene (PE), polypropylene (PP), polystyrene (PS), polyvinyl acetate (PVA) and poly (butylene succinate) (PBS))
Golzar et al. [488]
Binary VLE (CO2 and hydrogen sulphide in water and potassium carbonate) VLE of CO2 with single and mixed electrolyte solutions containing Na+, K+, Ca2+, Mg2+, Cl-, Br- and SO24 Quaternary VLE (CO2-water-hydrogen
Tang et al. [489] Jiang et al. [490]
Ji and Zhu [491] (continued on next page)
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Table 12 (continued) Solvent type
Model (chemical potential calculation) Gas-phase
System type
Ref.
Solvent-phase
Ion-based SAFT (SAFT2) EOS Homogenous approach Modified SAFT EOS with restricted primitive model (SAFT1-RPM) Homogenous approach Combination of Perturbed-Chain SAFT (PC-SAFT) EOS and Debye-Huckel term (ePC-SAFT) Homogenous approach PC-SAFT; Truncated PC-Polar SAFT (tPC-PSAFT) EOS Homogenous approach Extension of PPC-SAFT (ePPC-SAFT) EOS Homogenous approach Electrolyte-based extension of SAFT-VR (SAFT-VRE) EOS Homogenous approach SAFT-Lennard Jones (LJ) (SAFT-LJ) EOS
sulphide-sodium chloride) Binary (CO2-water) and ternary VLE (CO2-water-sodium chloride) VLE of CO2 and sulphur dioxide in brines at high pressures and temperatures Binary VLE of CO2 and water
Binary VLE (in 20 alkali-halide aqueous solutions) Binary VLE of CO2 in sodium chloride Ternary VLE (CO2-water-sodium chloride)
Ji et al. [492] Tan et al. [493]
Diamantonis and Economou [494] Rozmus et al. [495] Schreckenberg et al. [496] Sun and Dubessy [497]
Fig. 9. Status of original UNIFAC model group interaction parameter matrix using approach 3 for subgroup definition [506].
tural variations on the activity coefficient are not considered and a lot of parameters would be necessary to include an extensive list of cations [501]. Approach 2: This approach considers cation and anion skeletons as one entity [504]. It was credited by Lei et al. [501] for enabling the elimination of long-range electrostatic force term in activity coefficient calculation. However, if numerous cations and anions are to be considered, the parameter matrix would be very large. Approach 3: This approach separates each IL into a cation, an anion and their substituents (with imidazolium ion as a functional group) [505]. This approach is advantageous in the sense that it takes into account the impacts of structural variations of cation, anion and their substituents, and could result in the most compact parameter matrix. However, it would have highly extensive experimental data requirement for parameter regression. The existing IL-UNIFAC models extended for carbon dioxide solubility prediction (i.e. binary VLE) include original UNIFAC model and modified UNIFAC (Dortmund) model. For the original UNIFAC model, approach 2 was applied to regress interaction parameters for 22 ILs involving cations i.e. IM, PYR, PYRR, N and P ions, and
anions i.e. BF4, PF6, Tf2N, TfO, methylsulphate (MeSO4), ethylsulphate (EtSO4), chloride (Cl), diethylphosphate (DEPO4), dimethylphosphate (DMPO4), 2-(2-methoxyethoxy)ethylsulphate (MDEGSO4), NO3 and thiocyanate (SCN) ions [498]. In the associated modified UNIFAC (Dortmund) model, approach 3 was used but only involved ethyl (C2) - hexyl (C6) substituted methylimidazolium (MIM) cations and anions i.e. BF4, PF6 and Tf2N ions [482]. The group interaction parameter matrixes for original UNIFAC and modified UNIFAC (Dortmund) models applying approach 3 for subgroup definition are illustrated in Figs. 9 and 10, which are summarised based on the research outcomes of Hizaddin and Hadj-Kali [482], Kato and Gmehling [506], Nebig and Gmehling [507], Hector et al. [508], Paduszynski and Domanska [509], and Hector and Gmehling [510]. Despite being appealing in terms of compactness of interaction parameter matrix, they have not been extensively expanded for prediction of carbon dioxide solubility in ILs. More specifically, to date the modified UNIFAC (Dortmund) model developed by Hizaddin et al. [482] consists of five cations and three anions, and could only consider 15 possible IL combinations. In contrast, the ab initio
W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663
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Fig. 10. Status of modified UNIFAC (Dortmund) model group interaction parameter matrix using approach 3 for subgroup definition [482,506–510].
models have considered a more diverse array of ILs, as summarised in Table 13. Hence, UNIFAC model shall be extended to include these additional cationic and anionic species. Similarly, analogous UNIFAC model for prediction of ternary VLE phase equilibrium involving carbon dioxide, methane/hydrogen and ILs is still not existent. Specifically, relevant works included PR EOS model fitted by Ramdin et al. [511] for simulating ternary VLE of carbon dioxide/methane mixture with ILs, modified PR EOS developed by Shiflett et al. [512] and molecular simulation by Handy et al. [513] for separation of carbon dioxide from hydrogen sulphide via ILs, as well as soft SAFT EOS by Pereira et al. [514] and generic RK EOS by Shiflett et al. [515] for IL-based separation of carbon dioxide from nitrous oxide. It shall be noted that several important variants have been developed, and they are different from each other in terms of interaction parameter am;n formulations (with temperature as independent variable) and data type used for parameter regression. These UNIFAC variants are summarised in Table 14, whereby amn,0, amn,1, amn,2 denote regressed interaction parameters, T is temperature and T0 is room temperature.
7. Summary of research gaps In this section, potential research directions in the field of precombustion carbon capture and IL (as physical solvent) development are presented. For the former, research on the composite material or nanoparticle-based technology is required to optimise the stability of construction material against the corrosion issue and carbon fouling in the reformer section. In addition, future researchers
are also encouraged to find solutions for reducing the costs of carbon dioxide separation technologies, for instance by exploring the potential of more biomass materials, agricultural wastes and mine wastes for adsorbent (i.e. activated carbon and calcium oxide) synthesis. Functionalisation of MOF adsorbent material with multiple functional groups and metallic cations has also appeared as a new trend for improving the adsorption separation performance. In this particle field, focus shall also be put forward to the economics and availability assessment of the precious metals and raw ingredients. From the review of CAMD aspect, it has been identified that the current comprehensively developed IL-based UNIFAC models involve subgroup segmentation that results in bulky binary interaction parameter matrix, and therefore are inconvenient to use when cations and anions are to be chosen from comprehensive lists. Therefore, the UNIFAC model version considering cationic, anionic mainframe and substituent as separate subgroups (as in the work of Hizaddin et al. [482]) shall be further extended to include more IL constituents (i.e. phosphonium [P], ammonium [N], guanidinium [GUA] and morpholidinium [MOR]). To date, only original UNIFAC and modified UNIFAC (Dortmund) models have been extended for prediction of carbon dioxide solubility in ILs. KT-UNIFAC model, which has greater accuracy and could better describe the isomeric molecular difference of IL species, deserves further exploration for IL-based UNIFAC development. In addition, the current IL-based UNIFAC model should be extended to simultaneously simulate the VLE phase equilibrium of multiple gases (i.e. carbon dioxide/hydrogen and carbon dioxide/ methane) in a wider array of ILs for pre-combustion carbon capture solvent screening. This would be necessary for identification of functional groups sensitive to carbon dioxide/hydrogen and carbon dioxide/methane selectivities.
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Table 13 Coverage of ionic liquids in ab initio models. Solubility model
Description
Classes of ionic liquids (IL)
Ref.
COSMO-RS
12 cations and 6 anions; 72 ILs
Cation: imidazolium (IM), ammonium (N), phosphonium (P), and guanidinium (GUA); Anion: tetrafluoroborate (BF4), hexafluorophosphate (PF6), bis(trifluoromethylsulphonyl) imide (Tf2N), nitrate (NO3), triflate (TfO), and tris(pentafluoroethyl)trifluorophosphate (FEP) Cation: IM, PYR, PYRR, and sulphoniume (SUL); Anion: acetate, borate, phosphate/phosphinate, carbonate, salicylate, saccharinate, aluminate, acesulphamate, and cyanomethane Cation: IM, PYR, PYRR, N, P, quinolinium (Q), and isothiouronium (T); Anion: NO3, BF4, PF6, Tf2N, dicyanamide (DCA), thiocyanate (SCN), sulphonate, trifluoroacetate (TFA), and phosphate
Maiti [478]
212 cations and 63 anions; 13,356 ILs 170 ILs
Farahipour et al. [480] Palomar et al. [499]
COSMO-SAC
73 cations and 37 anions; 2701 ILs
Cation: IM, PYR, PYRR, N, P, GUA, PIP, souronium (U), T, Q, and aniline; Anion: acetate, borate, sulphonate, imide/amide, phosphate/phosphinate, and halogenide
Sumon and Henni [479]
Molecular simulation of hildebrand solubility parameters
21 cations and 10 anions; 210 ILs
Cation: IM, PYR, U, T, N, P, and GUA; Anion: acetate, sulphonate, Tf2N, TfO, phosphate, borate, PF6, and BF4
Sistla et al. [487]
8. Challenges of pre-combustion carbon capture technology 8.1. Commercial viability From global point of view, pre-combustion carbon capture technology has gained attention from the industrial players (especially coal and biomass gasification power plants) in the United States and European countries. However, this technology is still not widely commercialised worldwide since the enabling technologies (i.e. syngas-compatible industrial energy system, gas turbine system and fuel cell technology) are still largely at research stage. Therefore, the overall demand is far limited compared to postcombustion carbon capture technology. In Malaysia, hydrogen production technology (i.e. steam methane reforming and biomass gasification) is not practically existent despite having research progress to enable future application [529]. It shall be noted that most of the power plants in Malaysia being direct-fired type (either coal or biomass), which would be more compatible with post-combustion carbon capture system. Pre-combustion carbon capture system, on the other hand, is limited to new power plants since it has to be integrated from the conceptual design phase [45]. The local operating technological setting has inherently defied the need of pre-combustion carbon capture. Physical absorption using IL, on another part, poses another terrain of challenge for its commercialisation. In fact, despite having extensive modelling and simulation research works conducted on IL solvent design, IL has still not gained enough confidence level for commercialisation. 8.2. Financial constraint In terms of financial consideration, pre-combustion carbon capture system involves higher capital cost. For instance, capital expenditure of approximately USD 1169–1565/kW has to be invested for a single IGCC power plant with carbon capture, as reported by Thambimuthu et al. [44]. Furthermore, for existing power plants and other potential industrial sectors, its application would require a major retrofitting modification [45]. Moreover, the cost of ILs is prohibitively high for commercial usage, in contrast to the other conventional physical solvents, even if pre-combustion carbon capture is to be deployed.
At international scale, the existing driving forces i.e. IEA 2C limit and Kyoto treaties are all based on voluntary basis, and as such not seriously considered by the industrial and commercial players. In Malaysian scenario, there is no regulatory emissions limit for carbon dioxide, and carbon capture technology installation is not mandatory in contrary to the conventional air pollution abatement (for controlling the particulate matter, sulphur dioxide, carbon monoxide and nitrogen oxide emissions). According to Clean Development Mechanism (CDM) [530], termination of CDM programme at the end of 2012 had deprived all sustainability-related development projects of financial incentive through sales of certified emission reductions (CER) to the Europe’s Emissions Trading Scheme. This policy change would indirectly slow down the progress of CCS development among the local industrial players. 8.4. Technological constraint Despite already having several commercial-scale precombustion carbon capture facilities worldwide, there are still technical uncertainties in the operation and equipment design involved. For regions already implementing pre-combustion carbon capture, advanced technologies i.e. hydrogen turbine and acid gas shift conversion unit operation are highly complex, lacking reliability and vulnerable to unexpected accidents when upscaled to full commercial capacity [531]. Moreover, other technical problems comprise of fouling problem at reformer section (due to carbon deposition) and corrosion issue. Currently, research advancement for improving the operational efficiency, safety and health aspects of pre-combustion carbon capture technology is still in dire need. In Malaysia, obvious technical problem is the lack of professional technicians in Malaysia capable of monitoring the operation, troubleshooting and maintaining the CCS plant. Moreover, most of the advanced CCS technologies are still in laboratorial testing stage, and lack pilot, demonstration or full commercial-scale prototype for demonstrating their practical effectiveness. While reliance on the technology imported from foreign country would be prohibitively costly, slow research progress on CCS technology, lack of systematic analysis and updated technical information have made the research-to-commercialisation transition difficult.
8.3. Governance and regulatory framework 9. Future prospect of pre-combustion carbon capture Governmental incentives, long-term policies, CCS-based emission trading and regulatory framework, which are important to induce CCS investment, are lacking worldwide.
Despite the challenges above, pre-combustion system has high strategic significance due to flexible performance at large scale,
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W.L. Theo et al. / Applied Energy 183 (2016) 1633–1663 Table 14 Summary of UNIFAC model variants. UNIFAC variant
Temperature dependency of parameter
Data for parameter estimation
Comment
Ref.
Original UNIFACVLE
Independent of temperature
Vapour-liquid equilibrium (VLE)
Recommended over narrow range of temperatures
Fredenslund et al. [516]; Fredenslund et al. [500]; Hansen et al. [502]
Original UNIFAC-LLE
Independent of temperature
Liquid-liquid equilibrium (LLE)
Limited application due to narrow temperature range around room temperature
Magnussen et al. [517]
Linear UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE
–
Hansen et al. [518]
Modified UNIFAC (Lyngby)
Logarithmic dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, Enthalpy of mixing (HE)
Modification on combinatorial term
Larsen et al. [519]
Independent of temperature
VLE, Activity coefficient of infinite dilution (c1), Water data
Suited for calculation of octanolwater partition coefficient
Chen et al. [520]
Quadratic dependence:
VLE, LLE
Suitable for water-hydrocarbon systems
Hooper et al. [521]
VLE, HE, c1
Modification on combinatorial term, and regression of r and q parameters
Wedlich and Gmehling [522]; Gmehling et al. [523]; Gmehling et al. [524]; Gmehling et al. [525]
þ amn;2 ðTlnðTT0 Þ þ T T 0 Þ Water-UNIFAC
Water-UNIFAC
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2 Modified UNIFAC (Dortmund)
Quadratic dependence:
KT-UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, HE, c1
Involvement of first-order and second-order estimations to overcome the problem of proximity effect and isomerism
Kang et al. [526]
KT-NIST UNIFAC
Linear dependence: amn ¼ amn;0 þ amn;1 ðT T 0 Þ
VLE, HE, c1
Involvement of first-order and second-order estimations to overcome the problem of proximity effect and isomerism; Involvement of higher-quality data compiled; Higher reliable, accurate and robust property prediction
Kang et al. [527]
UNIFAC-CI Modified UNIFAC-CI
Independent of temperature Quadratic dependence:
VLE, Solid-liquid equilibrium (SLE)
Regression of group interaction parameters not available in UNIFAC model
Mustaffa et al. [528]
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2
amn ¼ amn;0 þ amn;1 T þ amn;2 T 2
high thermal efficiencies, and capability to synthesise saleable products (i.e. electricity, hydrogen, fuels with lower carbon footprint, and chemical commodities) within reasonable carbon constraint. Decreasing availability of fossil fuel resources would induce gradual development and acceptance of various hydrogen production technologies (especially steam methane reforming technology) [529] and coal-based IGCC technology [532]. This indirectly creates the supply-demand chain to drive the commercialisation of pre-combustion carbon capture. Similarly, IL, although being economically infeasible and less competitive, would be a promising substituent (or solvent blend constituent) in the future for its low environmental impact and highly tuneable solvent properties. 10. Conclusion In conclusion, pre-combustion capture technology serves as one of the technically feasible alternatives for carbon capture in natural gas treatment, combined cycle gas turbine power plant, and coal gasification utilisation sector. Much ongoing research works are still in need to ensure the transition of this technology from research phase to full-scale commercial plants worldwide, provided sufficient funding from the government and relevant international non-governmental organisations (NGO). For the side of IL development as co-solvent for pre-combustion capture purpose, various experimental and simulation works have been conducted in local and international research institutes. In terms of CAMD
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