Emission of some pollutants from biomass combustion in comparison to hard coal combustion

Emission of some pollutants from biomass combustion in comparison to hard coal combustion

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Journal of the Energy Institute xxx (2016) 1e10

Contents lists available at ScienceDirect

Journal of the Energy Institute journal homepage: http://www.journals.elsevier.com/journal-of-the-energyinstitute

Emission of some pollutants from biomass combustion in comparison to hard coal combustion  ski*, Patrycja Łechtan  ska, Olga Namiecin  ska Grzegorz Wielgosin Lodz University of Technology, Faculty of Process and Environmental Engineering, Wolczanska 213, 90-924 Lodz, Poland

a r t i c l e i n f o

a b s t r a c t

Article history: Received 9 November 2015 Received in revised form 14 June 2016 Accepted 21 June 2016 Available online xxx

In the last decade biomass combustion has become one of the most important elements in the fight against global warming. For the sake of climate or environment protection people cut out large stretches of forests and burn them down It is widely believed that the combustion of wood and biomass is completely safe and does not cause any danger to people and the environment. Unfortunately, this is only a half truth. In fact, with considerably lower emissions of sulfur dioxide (SO2) from biomass combustion, significant amounts of organic micro-pollutants are emitted, among which there are more toxic compounds like polycyclic aromatic hydrocarbons (PAHs) and polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs). The aim of this paper was to assess the real situation. Seven samples of biomass were investigated, i.e. rape straw, oak bark, firewood and wood pellets, shrub willow and rape cake. Pulverized hard coal samples were used for comparison. The aim of the study was to determine and compare the pollution emission factors (per unit mass of fuel) of carbon monoxide (CO), nitrogen oxide (NO) and the sum of hydrocarbons (as total organic carbon e TOC) generated in the process of biomass combustion. Further, we compared the results obtained for coal as well as the effect of process operating conditions (temperature; air flow) on the emission factors. The investigations were carried out in a laboratory chamber furnace at five different temperatures (from 700 to 1100  C) and at three different air flow rates providing an excess of oxygen. In many cases the determined emission indicators for biomass combustion were higher than for hard coal. © 2016 Energy Institute. Published by Elsevier Ltd. All rights reserved.

Keywords: Biomass Combustion Emission Laboratory tests

1. Introduction Biomass has been known and used by mankind as a fuel since ancient times. Today, it is particularly common, primarily as a fuel in poorer countries which lack other resources of fossil fuels, because it is a readily available and renewable solid fuel for heating and preparing meals. In recent years, biomass is increasingly used as a renewable fuel for heat and power generation on an industrial scale, replacing gradually depleting fossil fuels. On the other hand, the fact is that biomass is formed by the process of photosynthesis; plant organisms absorb carbon dioxide from the air and convert it into organic carbon, forming a basic timber which is thus a source of plant growth. This means that the combustion of biomass only releases carbon dioxide that has already been circulated in the atmosphere, without introducing new quantities. The advantages of biomass as a renewable energy source include primarily independence of the country in the sphere of supplies of fossil fuels and so-called “zero-emission” of CO2 during the combustion of biomass. Biomass is the third largest natural source of energy in the world. The total global potential of biomass is estimated at approx. 100e440 EJ/year, which represents approx. 30% of global energy demand. At the moment, for energy purposes approx. 40 EJ of energy from biomass is consumed per year [1e4]. Poland is a country with a climate conducive to energy crops and relatively rich in wood. The annual consumption of biomass for energy purposes is approx. 211.5 PJ with total primary energy demand of 4,480.1 PJ, which gives approx. 4.72% [5]. According to Directive 2010/75/EC of the European Parliament and Council on industrial emissions [6], the term biomass is understood as products consisting of any vegetable matter from agriculture or forestry which can be used as a fuel for the purpose of recovering its energy

* Corresponding author.  ski). E-mail address: [email protected] (G. Wielgosin http://dx.doi.org/10.1016/j.joei.2016.06.005 1743-9671/© 2016 Energy Institute. Published by Elsevier Ltd. All rights reserved.

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

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content and some waste (vegetable waste from agriculture and forestry, vegetable waste from the food processing industry, if the heat generated is recovered, fibrous vegetable waste from virgin pulp production and from production of paper from pulp, if it is co-incinerated at the place of production and the heat generated is recovered, waste cork and wood waste with the exception of wood waste which may contain halogenated organic compounds or heavy metals as a result of treatment with wood preservatives or coating, and which includes in particular such wood waste originating from construction and demolition waste). On the other hand, Directive 2009/28/EC of the European Parliament and Council on the promotion of energy from renewable sources and amending and subsequently repealing Directives 2001/77/ EC and 2003/30/EC [7] defines biomass as the biodegradable fraction of products, waste and residues (including vegetal and animal substances), forestry and related industries including fisheries and aquaculture, as well a biodegradable fraction of industrial and urban areas. Biomass, as a fuel has several advantages among which the most important are its availability, renewability and “zero-emission” of CO2. However, apart from several advantages as an energy source material, it has also some disadvantages, among which are [8e11]: -

Relatively low density of raw materials, hindering the transport, storage and dispensing, Wide range of biomass humidity, which makes it difficult to prepare for use for energy purposes, Lower than for fossil fuels energy value of raw material, Variability of fuel properties, resulting from changes in humidity and composition.

Biomass utilization for energy e heat and power production e is a subject of numerous studies and many publications in recent years. They cover both the combustible properties of biomass [12e15] and energy generation technologies. Direct combustion [16e19] and cocombustion with coal [20e25] is the well-known oldest way of using biomass as a source of energy [26,27]. Biomass thermo-chemical conversion technologies such as pyrolysis and gasification are certainly not the most important options at present; combustion is responsible for over 97% of the world's bio-energy production [12]. However, co-firing of biomass and coal (both bituminous and subbituminous coal and lignite) has technical, economical, and environmental advantages over the other options. Technical issues that can lead to doubt about of biomass co-firing with coal are being resolved through testing and experience [28]. The main current biomass technologies include [29e32]: -

Destructive carbonization of woody biomass to charcoal, Gasification of biomass to gaseous products, Pyrolysis of biomass and solid wastes to liquid, solid and gaseous products, Supercritical fluid extractions of biomass to liquid products, Liquefaction of biomass to liquid products, Hydrolysis of biomass to sugars and ethanol, Anaerobic digestion of biomass to gaseous products, Biomass power for generating electricity by direct combustion or gasification and pyrolysis Co-firing of biomass with coal, Biological conversion of biomass and waste (biogas production, wastewater treatment), Biomass densification (briquetting, pelleting), Domestic cook stoves and heating appliances of fuel wood, Biomass energy conservation in households and industry, Solar photovoltaic and biomass based rural electrification, Conversion of biomass to a pyrolytic oil (biofuel) for vehicle fuel, Conversion of biomass to methanol and ethanol for internal combustion engines.

However, despite the possibility of such large biomass conversion and utilization technologies, its simple combustion or co-combustion with coal still dominates [29]. Combustion is a complex phenomenon involving simultaneous coupled heat and mass transfer with chemical reaction and fluid flow. Its chemistry can be described by the following reaction scheme, where the simplified chemical structure of biomass is presented as a first reactant [13]:

Cx1 Hx2 Ox3 Nx4 Sx5 Clx6 Six7 Kx8 Cax9 Mgx10 Nax11 Px12 Fex13 Alx14 Tix15 þ n1 H2 O þ n2 ð1 þ eÞðO2 þ 3; 76N2 Þ

/

Combustion

n3 CO2 þ n4 H2 O þ n5 O2

þ n6 N2 þ n7 CO þ n8 CH4 þ n9 NO þ n10 NO2 þ n11 SO2 þ n12 HCl þ n13 KCl þ n14 K2 SO4 þ n15 C þ … It is evident that biomass combustion process will be accompanied by the emission of many pollutants. Primary pollutants formed are particulate matter (PM), carbon monoxide (CO), hydrocarbons (HC), oxides of nitrogen (NOx, principally NO and NO2), and oxides of sulfur (SOx, principally as SO2). Acid gases, such as hydrochloric acid (HCl), may also be emitted, as may lead and other heavy metals. CO and HC, including volatile organic compounds (VOC) and polycyclic aromatic hydrocarbons (PAH), are products of incomplete combustion [33]. These species are largely controlled by stoichiometry and proper fuel moisture control. Biomass has a significantly lower heating value than most coal. This is in part due to the generally higher moisture content and in part due to the high oxygen content. It was observed that the investigated biomass materials showed different combustion characteristics. Results of the structural, proximate and ultimate analyses of biomass and wastes differ considerably. And of course we must remember that coal and biomass fuels are quite different in elemental composition and combustion properties. The greatest advantage of biomass is that it is a renewable fuel. The application of biomass as a fuel would increase energetic safety and stability in the market of fuels and energy [34,35]. Nonetheless, up to the present, no technology has been developed which allows energy to be acquired 100% ecologically. This is because the processing of raw materials, (either non-renewable or renewable) is connected with a smaller or larger impact on the particular environmental components (the air, water, soil, etc). All precautions are taken so that the negative  ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

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consequences are minimal while, at the same time, achieving the highest energy efficiency and maximizing financial profits. Biomass is in the third position as regards the natural energy source. It is also one of the longest utilized energetic raw materials because wood combustion has been a known method of generating heat since the dawn of civilization. It is the main source of domestic energy in the developing world (especially in under-developed countries) both for the production of heat and power [36e42]. Biomass is commonly considered to be an ecological fuel. In recent years, a large number of investigations have been carried out with the aim of checking the thesis, in particular with reference to pollutant emissions [43e55]. The general conclusions are as follows: cocombustion of biomass may decrease the emission of certain pollutants e particularly of sulfur dioxide and nitrogen oxides, but it may cause increased emission of carbon monoxide and other products of incomplete combustion, including polycyclic aromatic hydrocarbons (PAH) [56e58] and polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) [59e67]. The aim of the present study was to compare the emission indicators of such pollutants as carbon monoxide (CO), nitrogen monoxide (NO) and the sum of hydrocarbons (as the total organic carbon TOC) generated in the process of combustion of seven types of biomass and using fine coal as the reference fuel. The purpose of this paper is to draw attention to the problem of emissions from the combustion of biomass compared to coal combustion. 2. Materials and methods The aim of the study was to determine the indicators of emission of carbon monoxide, nitrogen monoxide and the sum of hydrocarbons per unit mass of combusted fuel for the following seven types of biomass: -

Basket willow e Salix viminalis (chips), Rape straw (briquette), Wood waste from a forest (pellets), Poplar firewood (chips), Sawdust from a joinery, Oak bark (shavings, taken from a sawmill), Rape cake

as well as to compare them with the indicators determined for fine coal combustion under identical conditions as biomass and to determine the influence of combustion conditions (temperature, air flow) on the emission of the aforementioned pollutants. The basic properties e moisture content, organic substance content (in dry matter), ash content (in dry matter), of the examined samples according to our own notation e are summarized in Table 1. Investigations of the combustion process were carried out in an electric resistance furnace e pipe furnace with a horizontal working chamber of the type PR-45/1350-M equipped with a programmable temperature regulator PRT 911, enabling to maintain the temperature set at a given time (produced by the Industrial Institute of Electronics, Warsaw). The analysis of carbon monoxide (CO) and nitrogen oxide (NO) concentrations in gases originating from the combustion process was made using a GA-20 flow analyzer of flue gases (EL-Jack Madur Electronics, Zgierz), whereas the analysis of total hydrocarbons (as Total Organic Carbon e TOC) was carried out using an AWE-S flame ionization detector (FID) analyzer cooperating with a WHR-1 hydrogen generator (Research and Design Company LAT, Katowice). The experimental setup is shown schematically in Figs. 1 and 2. Investigations of the combustion process were carried out for the following parameters: - Combustion temperature: 700  C, 800  C, 900  C, 1,000  C, 1,100  C. - Air flow rate: 4 dm3/min (0.0000667 m3/s), 9.1 dm3/min (0.000152 m3/s), 14.7 dm3/min (0.000245 m3/s). The test procedure was as follows e after reaching the predetermined temperature in the combustion furnace at a set air flow a quartz boat with sample material was introduced into the combustion zone and the combustion started. In that moment the recording of emissions began. After about 5 min the concentration of tested pollutants in the exhaust stream decreased to zero at which point the experiment was terminated. The recorded concentrations were used to calculate the emission factor, i.e. the amount of the total emission recorded by the instrument, referred to the mass of combusted samples. To determine the concentrations of CO and NO an electrochemical analyzer was used, while for TOC indications e flame ionization detector (FID). It was not our goal to study the kinetics of combustion and to determine emission factors for the purpose of emission inventories, hence the simple devices for CO and NO measurement (electrochemical) were used. All emission curves were recorded starting

Table 1 Basic properties of the investigated biomass and coal. Sample

Moisture content

Organic substances content

Ash content

%

% D.M.

% D.M.

Straw Bark Sawdust Fire-wood Pellet Willow Rape cake Coal

8.02 8.33 8.07 8.48 7.48 26.87 7.82 6.52

95.33 95.46 99.62 98.54 94.62 97.42 92.27 98.05

4.67 4.54 0.38 1.46 5.38 2.58 7.73 1.95

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

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Fig. 1. Scheme of an experimental setup for the investigation of CO and NO emission.

Fig. 2. Scheme of an experimental setup for the investigation of TOC emission.

from the time when samples were introduced into the combustion zone until the moment where no emission occurred, so the time constant of the analyzer was insignificant. It was important to burn all samples in the same conditions. Due to non-homogeneity of the research material, it was necessary to repeat measurements a number of times under identical conditions. Measurements of CO and NO were carried out three times and of TOC five times. A mean emission value was calculated from the results obtained. Typical emission curves for particular pollutants can be seen in Figs. 3e5. The values of emission factor (in mg pollutant per gram of combusted fuel) for particular pollutants were derived from the following equation:

wz ¼

Q $csr $t mp

where: Q e flow rate of air supplied for combustion [m3/s] mp e mass of the fuel sample [g] t e time of sample combustion [s] csr e mean pollutant concentration during combustion [mg/m3] calculated from the following expression:

csr ¼

1

t

Zt

cðtÞdt

0

CO [ppm] 3500 3000 2500 2000 1500 1000 500 0 0

50

100

150

200

250

300

350

400

450

500

550

600

time [s] Fig. 3. Example of the dependence of CO emission on time.

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

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NO [ppm] 90 80 70 60 50 40 30 20 10 0 0

50

100

150

200

250

300

350

400

450

500

550

600

time [s] Fig. 4. Example of the dependence of NO emission on time.

TOC [ppm] 450 400 350 300 250 200 150 100 50 0 0

50

100

150

200

250

300

350

400

450

500

550

600

time [s] Fig. 5. Example of the dependence of TOC emission on time.

In all conditions of the combustion process, all investigated samples were combusted in a considerable excess of air. The procedure for determination of the emission indicators during combustion was described in detail in an earlier publication [68].

3. Results and discussion For each sample of the seven types of biomass and coal the combustion tests were performed at all selected temperatures and three differing air flow rates. The emission indicator, taken as the amount of a pollutant generated on combustion (mg: CO, NO, TOC) per unit mass (1 g) of combusted fuel, was determined for each sample. The dependence of the emission indicator on the combustion temperature for various values of the volumetric air flow rate for all the investigated biofuels and coal was calculated. Figs. 6e8 show the dependence of the carbon oxide emission indicator on the conditions of the combustion process. Figs. 9e11 illustrate the analogous dependence for the nitrogen oxide emission indicator and Figs. 12e14 show the dependence of the emission indicator on the sum of organic compounds denoted as total organic carbon (TOC). Analyzing the results, we observe that biofuels require better aeration of the combustion zone than hard coal e this is particularly visible at elevated temperatures. It is reflected by a clear increase of the CO emission indicator for all the investigated biofuels at temperatures >900  C (Fig. 6). At 700  C the CO emission indicator for fine coal is higher than for biofuels. Generally, among biofuels the highest CO emission indicator is observed for straw, whereas the lowest one for willow. In the case of nitrogen oxide emission at 700  C the lowest emission indicator is obtained for coal, however, as the temperature rises, the value of the NO emission indicator for coal increases attaining values higher than for biofuels, but at 1,100  C it drops abruptly. The biggest NO emission is observed for rape cake, which is twice as high as for other biofuels. It is highly probable that the higher values of the NO emission indicator for coal result from the considerably higher calorific value of this fuel in relation to biomass, resulting in the generation of transiently very high temperatures in the combustion zone and the intensive nitrogen oxide synthesis in accordance with the thermal mechanism by Zeldowich. Nonetheless, on the whole, the NO emission decrease at the highest temperature was observed for all the fuels examined. This decrease is the smallest at the lowest air flow rate. One may suppose that this is a result of alterations in the course of NO synthesis under these conditions. The highest nitrogen oxide emission indicators generally appear for coal combustion. Among biofuels, the highest and lowest emission indicators were attained for straw and willow combustion, respectively.  ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

Fig. 6. Dependence of CO emission indicator on temperature for Q ¼ 4.0 dm3/min.

Fig. 7. Dependence of CO emission indicator on temperature for Q ¼ 9.1 dm3/min.

Fig. 8. Dependence of CO emission indicator on temperature for Q ¼ 14.7 dm3/min.

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

Fig. 9. Dependence of NO emission indicator on temperature for Q ¼ 4.0 dm3/min.

Fig. 10. Dependence of NO emission indicator on temperature for Q ¼ 9.1 dm3/min.

Fig. 11. Dependence of NO emission indicator on temperature for Q ¼ 14.7 dm3/min.

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

Fig. 12. Dependence of TOC emission indicator on temperature Q ¼ 4.0 dm3/min.

Fig. 13. Dependence of TOC emission indicator on temperature for Q ¼ 9.1 dm3/min.

Fig. 14. Dependence of TOC emission indicator on temperature for Q ¼ 14.7 dm3/min.

 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005

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Practically, in every combustion conditions the emission indicator of total organic compounds was the lowest for coal combustion but for biofuels it attained higher values. Similarly to the former emission indicators and in the case of total organic compounds the highest values of the emission indicator were obtained for straw and pellets but the lower ones for willow and bark. Initially, this indicator decreased and then it increased with the increase of temperature attaining the minimum at a temperature of 800e900  C. This is a very unfavorable phenomenon because it is the evidence that organic compounds are synthesized at elevated temperatures from organic radicals present in the combustion zone. These steps include cyclization, i.e. the creation and ring closure of aromatic compounds and also chlorination and dioxin synthesis. Gaseous chlorine is practically always present in the combustion zone because all fuels, including biomass, contain small quantities of chlorine. In the case of coal combustion, dioxin synthesis takes place at high temperatures and to a smaller extent due to the inhibitory influence of sulfur present in coal. In the case of biofuels the amount of sulfur is considerably lower and, therefore, emission of dioxins and furans may be expected. This conclusion is confirmed by recent works on wood combustion [59,60,66]. 4. Conclusions The combustion of seven biomass types (basket willow S. viminalis chips, rape straw briquettes, pellets of rape cake and sawdust, firewood chips, oak bark) was investigated. In many cases, the determined emission indicators, in particular of total organic compounds, are unexpectedly higher than for hard coal. Thus, it is difficult to consider biomass as a truly ecological fuel. Although it is undoubtedly a renewable fuel it is not ecological. The intensity of its emissions is far too high and comparable to those in coal combustion, while hydrocarbon emissions are even higher. 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 ski, et al., Emission of some pollutants from biomass combustion in comparison to hard coal Please cite this article in press as: G. Wielgosin combustion, Journal of the Energy Institute (2016), http://dx.doi.org/10.1016/j.joei.2016.06.005