J. Chem. Thermodynamics 95 (2016) 136–141
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Solubility and viscosity for CO2 capture process using MEA promoted DEAE aqueous solution Dong Fu ⇑, LeMeng Wang, Pan Zhang, ChenLu Mi School of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, People’s Republic of China
a r t i c l e
i n f o
Article history: Received 19 August 2015 Received in revised form 24 November 2015 Accepted 2 December 2015 Available online 14 December 2015 Keywords: Solubility Viscosity CO2 DEAE MEA
a b s t r a c t The saturated solubility of CO2 in monoethanolamine (MEA) promoted 2-diethylaminoethanol (DEAE) aqueous solution was investigated at temperatures ranging from (303.2 to 323.2) K. The mass fraction and temperature dependences of the saturated solubility and CO2 loading are illustrated. The viscosities of both CO2-unloaded and CO2-loaded DEAE–MEA aqueous solutions were measured and then calculated by using the Weiland equation. The effects of temperature, mass fraction and CO2 loading on viscosities are demonstrated. Ó 2015 Elsevier Ltd. All rights reserved.
1. Introduction The greenhouse effect and the acid rain caused by the emissions of carbon dioxide (CO2) have attracted increasing attentions worldwide and the reduction of CO2 has become a global issue [1–3]. Many technologies, including chemical absorption, physical adsorption, membrane separation, oxygen combustion of fuel [4,5], are currently employed for the separation of CO2 from gas streams. Among these technologies, amine-based absorption technologies are considered to be the most robust and able to be used on a large scale for post-combustion CO2 capture [6–8]. Alkanolamines, such as monoethanolamine (MEA), diethanolamine (DEA) and N-methyldiethanolamine (MDEA), have been widely applied to remove the acid gases in industrial processes [6,9]. In recent decades, interest increased rapidly in the use of mixed amine absorbents, especially the blends of primary-tertiary amines (e.g., MEA–MDEA) or secondary-tertiary amines (e.g., DEA–MDEA). The blending amines combine the high equilibrium capacity and low enthalpy of the tertiary amine with the high reaction rate of the primary or secondary amine [10,11]. The primary or secondary amine plays a role as activator. For example, MEA is considered as the promising additive to MDEA aqueous solution because it can absorb CO2 and forms intermediate very quickly, and then the intermediate transfers CO2 to MDEA [12]. Thus, small amount of MEA can significantly accelerate the absorption rate of CO2 in ⇑ Corresponding author. Tel.: +86 312 7522037; fax: +86 312 7523127. E-mail address:
[email protected] (D. Fu). http://dx.doi.org/10.1016/j.jct.2015.12.001 0021-9614/Ó 2015 Elsevier Ltd. All rights reserved.
MDEA aqueous solution under appropriate temperatures. By far, adding small amount of MEA to an aqueous solution of MDEA has found widespread application in the removal of CO2 [13–17]. The absorption performance of MEA-tertiary amine aqueous solution depends on the characteristics of both MEA and tertiary amine, e.g., high reaction rate of MEA, high cyclic capacity and low enthalpy of tertiary amine. Development of new absorbents with higher absorption rates, higher absorption capacities, higher cyclic capacities and lower reaction enthalpies has attracted great attention for reducing CO2 emission. Recently, Chowdhury et al. [18] investigated the absorption characteristics of 24 tertiary amine absorbents and compared their performances with that of the conventional tertiary absorbent MDEA. Via laboratory experiments, seven tertiary amines with potential application in CO2 capture were screened out. In particular, amine 2-diethylaminoethanol (DEAE) shows good chemical stability, higher CO2 loading capacities, higher cyclic capacities yet lower heats of reaction than MDEA. Puxty et al. [19] studied the CO2 absorption performance in 76 amines including DEAE. The trend of initial CO2 absorption rate was given as DEAE > MDEA. By far, there are many studies concerning the thermodynamics and kinetics of solutions containing DEAE. Lebrette et al. [20] and Maham et al. [21] investigated the volumetric properties of DEAE aqueous solutions over the entire composition range at different temperatures. Benitez-Garcia et al. [22] measured the effect of basicity on the absorption of CO2 in tertiary amines aqueous solution at T = 298 K. Kim and Savage [23] studied the absorption rates of CO2 in DEAE aqueous solutions at 323 K and showed that the
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second-order kinetic rate constant increased with increasing basicity. Xu et al. [24] used 1,4-butanediamine (BDA) promoted DEAE aqueous solution to capture CO2 and found that the addition of BDA into DEAE aqueous solution did accelerate the absorption rate. Littel et al. [25] investigated the kinetics of the absorption of CO2 in DEAE aqueous solutions at T = (293 to 333) K, and deduced that the reaction order is around 1.0 for all the investigated temperatures. Vaidya and Kenig [26] studied the absorption rate of CO2 in PZ promoted DEAE aqueous solutions at T = (298 to 308) K. Their results showed that small amount of PZ can significantly enhance the absorption rate. Konduru et al. [27] studied both the equilibrium and kinetic characteristics of the carbonated DEAE-PZ aqueous solutions. They concluded that CO2–DEAE–PZ system belongs to the fast pseudo-first-order reaction regime system and determined the second-order rate constant. Besides the absorption rate, the solubility of CO2 is also an important parameter for the estimation of the absorption capacity of absorbent. However, studies concerning the saturated solubility of CO2 in MEA–DEAE aqueous solutions under wide temperature and concentration ranges are rarely reported by far. Moreover, the solubility of CO2 is closely related to solution viscosity, because viscosity significantly affects the liquid film coefficient for mass transfer [14,28–30]. Previous work [31,32] showed that the addition of activator into amine aqueous solution +sometimes leads to abnormalities in absorption capacity, especially in the case of high solution viscosity, because high viscosity of the solution leads to a less diffusion coefficient of the gas in the solution, thus hinders the absorption. From these views, it is very necessary to study the viscosities of MEA–DEAE aqueous solutions and illustrate the effect of viscosity on the solubility and CO2 loading capacity. The viscosities of binary solutions of DEAE and water have been measured and the results over comprehensive ranges of compositions and temperatures have been reported in the literatures [20,21,33]. However, the studies concerning the viscosities of carbonated DEAE–MEA aqueous solutions are rare so far. The main purposes of this work are (1) to determine experimentally the solubility of CO2 in MEA promoted DEAE aqueous solution and illustrate its mass fraction dependence; (2) to determine experimentally the viscosities of carbonated DEAE–MEA aqueous solution and then calculate it with Weiland equation [34], so as to demonstrate the effects of temperature, CO2 loading, mass fractions of DEAE and MEA on viscosity. 2. Experimental 2.1. Materials DEAE and MEA were used without further purification. The sample description is shown in table 1. Aqueous solutions of DEAE–MEA were prepared by adding the high purity water made from the Heal Force ROE (Reverse Osmosis Electrodeionization)100 apparatus. 2.2. Apparatus and procedure The solubility was measured by the equipment composed of one high-pressure CO2 tank, one mass flow controller (MFC), one
mass flow meter (MFM), one absorption bottle, one constant temperature water bath, one desiccator and one CO2 analyzer (Advanced Gasmitter by Germany Sensors Europe GmbH, the accuracy is ±2%). The schematic diagram of the experiment is shown in figure 1. The flask was immersed into the thermostatic bath and the temperature of the solution can be regulated within 0.1 K. During the experiment, CO2 from a high-pressure tank (concentration C0 P 0.9999, temperature T0) was inlet into the MFC to maintain a constant flow rate (v0) and then into the absorption bottle and absorbed by the solution. The residual and unabsorbed gas firstly flowed into the CO2 analyser (temperature T1) and then into the mass MFM. The CO2 concentration (Ci) was measured by the CO2 analyser, and the flow rate (vi) was measured by the MFM. Ci, vi and the corresponding time ti were simultaneously recorded by the computer (interval time Dt = 1 s). The solution was saturated when Ci is close to 100%. The volume (V) of the absorbed CO2 can be calculated from:
V ¼ v 0 C 0 t273:15=T 0
X
v i C i Dt273:15=T 1
ð1Þ
i¼1
in which t is the total absorption time. The CO2 solubility can be calculated from:
n¼
V=22:4 44 100 m
ð2Þ
in which m is the total mass of CO2 unloaded DEAE–MEA aqueous solution. To verify the reliability of the equipment, the saturated CO2 loading in MEA aqueous solution (30 wt%, 0.1 MPa, T = 313.2 K) was measured. The uncertainties for temperature, wMEA, pressure and CO2 loading are respectively 0.1 K, 0.0001, 5 kPa and 0.03 molCO2 per molMEA. Our result (a = 0.58) is close to the value (a = 0.59) reported in the work of Shen et al. [37]. We also measured the CO2 loading in DEAE aqueous solution (61 wt%, 0.1 MPa, T = 313.2 K) and compared with the value reported in the work of Arshad et al. [38] (61.087 wt%, 97 kPa, T = 313.15 K). The uncertainties for temperature, wDEAE, pressure and CO2 loading are respectively 0.1 K, 0.0001, 5 kPa and 0.03 molCO2 per molDEAE. The deviation between our result (a = 0.76) and that from the work of Arshad et al. [38] (a = 0.798) is 5%. Once the carbonated solution was prepared, varying proportions of the unloaded and loaded solutions were mixed together to produce a set of samples. CO2 loading is defined as a ¼ nCO2 =ðnDEAE þ nMEA Þ [34,39], in which nCO2 is the mole of loaded CO2, and nDEAE and nMEA are respectively the moles of DEAE and MEA in the unloaded aqueous solutions. A certain amount of CO2 escaped when the loaded solution was mixed with the unloaded solution and the atmospheric CO2 and humidity had some effects on the CO2 loading and solution concentration. The CO2 loadings of some diluted samples were checked by using the analytical method based on the precipitation of BaCO3 [14,40]. The estimated uncertainty in the CO2 loading was less than 2%. The viscosities of the carbonated DEAE–MEA aqueous solutions were measured by using the NDJ-5S digital rotational viscometer produced by Shanghai Changji Geological Instrument factory. The measurement ranges and measurement error are respectively (0.1 to 105) mPa s and ±1% (for a Newtonian fluid).
TABLE 1 Sample description. Substance
Source
Mole fraction purity (as stated by the supplier)
CAS No.
Density/(g cm3) at T = 303.15 K
MEA DEAE Carbon dioxide Water
Aladdin reagent Aladdin reagent Jinglian Gas Heal force ROE-100apparatus
x P 0.995 x P 0.99 x P 0.9999 Electrical resistivity > 15 MX cm at T = 298 K
141-43-5 100-37-8
1.0077 [35] 0.87575 [36]
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FIGURE 1. Schematic diagram for experiments.
3. Results and discussion 3.1. Solubility and CO2 loading Values of the saturated solubility and CO2 loadings are shown in table 2. One may find from this table that at given mass fractions of DEAE (wDEAE) and MEA (wMEA), both the saturated solubility and CO2 loading decrease with increasing temperature. However, compared with the temperature dependence of solubility, the mass fraction dependence is more complex. Generally, the absorption of gas A in aqueous solution B may be formulated as:
pffiffiffiffiffiffiffiffiffiffiffiffiffiffi N / C A a DA kC B
ð3Þ
in which CA and CB are respectively the concentrations of gas A and absorbent B; DA, k and a are respectively the diffusion coefficient of gas A, the kinetic constants of the reaction and the absorbing surface area. The DA is dominated by the viscosity of the aqueous solution and according to the Othmer method [41], it can be formulated as following:
D 105 ¼
14
ð4Þ
gwater ð1:1 Ls =Lw ÞV 0:6 m g
in which Lw and Ls are respectively the latent heats of the vaporization of water and solvent. The gwater and g are respectively the viscosities of water and the aqueous solution, Vm is the molar volume of the diffusing substance. Combining equation (3) with equation (4) leads to:
N / ½kC B =g1:1
0:5
ð5Þ
Equation (5) quantitatively expresses the contributions of both mass fraction of absorbent and viscosity of the aqueous solution to the absorption, indicating both CB and g affect the absorption process and there exists competition between CB and g. As the increase of the mass fractions of amine and activator may induce a higher solution viscosity and a less diffusion coefficient of the gas in the solution, one may observe the conflicting influence of wMEA on the saturated solubility in some particular cases. For example, at wDEAE = 0.3, the saturated solubility of CO2 increases with the increase of wMEA. However, at wDEAE = 0.4, irregular influence of wMEA on the saturated solubility may be found in table 2, especially in the case of wMEA equal to 0.05. The wMEA dependence of the saturated CO2 loading is similar to that of saturated solubility, despite that the saturated CO2 loading decreases with the increase of wMEA, e.g., in the cases of wDEAE = 0.3 and T = 303.2 K,
TABLE 2 Solubilities (n) of CO2 in DEAE–MEA aqueous solutions and the corresponding CO2 loadings (a). p = 0.1 MPa. wDEAE
wMEA
a/(molCO2 per{mol DEAE + mol MEA})
n/(gCO2 per100 g aqueous solution) T = 303.2 K
T = 313.2 K
T = 323.2 K
T = 303.2 K
T = 313.2 K
T = 323.2 K
0.2999
0.0000 0.0501 0.0999 0.1501
9.84 10.11 11.54 12.76
9.52 9.78 10.81 12.32
9.23 9.19 10.15 11.39
0.87 0.68 0.63 0.58
0.85 0.66 0.59 0.56
0.82 0.62 0.55 0.52
0.4001
0.0000 0.0501 0.1001 0.1499
12.51 12.26 13.63 14.31
12.28 11.97 12.99 14.11
12.01 11.22 12.17 13.28
0.84 0.66 0.61 0.56
0.82 0.64 0.58 0.54
0.80 0.60 0.55 0.51
Standard uncertainties u are u(T) = 0.1 K; u(w) = 0.0001; u(p) = 5 kPa; u(a) = 0.03 molCO2 per {mol DEAE + mol MEA}, u(n) = 0.33 gCO2 per 100 g aqueous solution; wDEAE and wMEA are the initial mass fractions in the CO2-unloaded solutions.
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when wMEA increases from 0 to 0.15, CO2 loading decreases from 0.87 to 0.58.
TABLE 4 Viscosities of CO2-unloaded DEAE–MEA aqueous solutions. p = 0.1 MPa.
g/(mPa s)
wDEAE
wMEA
313.2 K
323.2 K
0.3001
0.0499 0.1001 0.1501
4.10 5.30 5.85
3.04 3.81 4.31
2.27 2.83 3.25
0.3499
0.0501 0.0999 0.1501
5.16 6.07 7.05
3.72 4.36 4.97
2.77 3.38 3.83
0.4001
0.0499 0.1001 0.1499
5.86 6.87 8.17
4.38 4.85 5.43
3.29 3.67 4.12
0.4501
0.0501 0.1001 0.1501
7.07 8.04 10.30
5.09 5.47 6.39
3.74 3.89 4.66
3.2. Viscosity and the model
T = 303.2 K
Values of the viscosity of CO2-unloaded DEAE aqueous solutions, CO2-unloaded and CO2-loaded DEAE–MEA aqueous solutions are shown in tables 3–6. The viscosities of CO2-unloaded DEAE aqueous solutions (wMEA = 0) from this work were compared with those from literatures [21,33,36,42]. Comparison shows that the average relative deviation between our values and those from available literature sources is less than 4%. Besides experiments, equations that can correctly correlate the viscosities are also important. Compared with the widely used Eyring equation [43] and the Grunberg–Nissan equation [44], the Weiland equation [34] can simultaneously describe the temperature, mass fraction of amine and CO2 loading dependences. Thus in this work, the Weiland equation [34] was applied to correlate the viscosities of both CO2-loaded and CO2-unloaded solutions. When applied to carbonated DEAE–MEA aqueous solutions, the Weiland equation can be expressed as:
gmix ¼
w1 w1 g þ g w1 þ w2 1 w1 þ w2 2
ð6Þ
where gmix is the viscosity of the carbonated aqueous solution, and w1 and w2 respectively stand for the mass fractions of DEAE and MEA, g1 and g2 are expressed as:
gi =gwater ¼ exp
½ðai w þ bi ÞT þ ðci w þ di Þw T2
f ða; wÞ
TABLE 5 Viscosities of CO2-loaded DEAE-MEA aqueous solutions. wDEAE = 0.30, p = 0.1 MPa. wDEAE/wMEA
a
313.2 K
323.2 K
0.2999/0.0501
0.10 0.20 0.30 0.40 0.50
f ða; wÞ ¼ aðei w þ f i T þ g i Þ þ 1
5.06 5.40 5.61 5.84 6.19
3.64 3.97 4.13 4.26 4.54
2.84 3.03 3.31 3.54 3.79
0.3001/0.1001
0.10 0.20 0.30 0.40 0.50
5.83 6.52 6.96 7.36 8.00
4.15 4.67 4.98 5.34 5.75
3.42 3.83 4.03 4.13 4.28
0.3001/0.1501
0.10 0.20 0.30 0.40 0.50
7.04 8.16 9.11 10.40 11.50
4.81 5.68 6.42 7.31 8.08
3.90 4.44 4.85 5.26 5.82
ð8Þ
where ai , bi , ci , di , ei , f i , g i are adjustable parameters. In this work, the model parameters of MEA, a2 = 0.0, b2 = 0.0, c2 = 21.186, d2 = 2373, e2 = 0.01015, f2 = 0.0093 and g2 = 2.2589, were directly taken from the previous work [12,34]. It is worth noting that the viscosity of DEAE aqueous solution does not increases monotonously with the increase of the mass fraction of DEAE (wDEAE). With increasing wDEAE, the viscosity shows a trend of first increase and then decrease. The Weiland equation cannot correctly describe such an irregular change of viscosity. Hence in this work, the parameters of DEAE were regressed by fitting to the viscosities of both CO2-unloaded and CO2-loaded DEAE–MEA aqueous solutions. The objective function is expressed as: n X ½1 gcal =gexp 100%=n
ð9Þ
Standard uncertainties u are u(T) = 0.1 K; u(w) = 0.0001; u(p) = 5 kPa; u(g) = 0.11 mPa s (g 5 10 mPa s); u(g) = 0.16 mPa s (10 mPa s < g); wDEAE and wMEA are the initial mass fractions in the CO2-unloaded solutions.
TABLE 6 Viscosities of CO2-loaded DEAE–MEA aqueous solutions. wDEAE = 0.40, p = 0.1 MPa. wDEAE/wMEA
a
T = 303.2 K
T = 313.2 K
T = 323.2 K
0.3001 0.3499
2.96,2.82 [21], 2.899 [33], 2.9 [36] 3.34, 3.61 [42]
2.12, 2.016 [21], 2.07 [36] 2.36, 2.42 [42]
0.4001 0.4501
4.56, 4.364 [21] 5.06, 5.269 [33], 5.23 [36]
3.12, 2.912 [21] 3.65, 3.50 [36]
0.4999 0.6001
6.11, 6.361 [21], 6.216 [33] 8.41, 8.984 [21], 8.687 [33], 8.05 [42]
4.33, 4.179 [21] 5.52, 5.497 [21], 5.27 [42]
1.59, [36] 1.81, [42] 2.23 2.69, [36] 3.07 3.74, [42]
7.02 8.07 9.53 10.8 12.7
5.07 5.65 6.48 7.31 8.24
3.83 4.24 4.69 5.23 5.95
0.4001/0.1001
0.10 0.20 0.30 0.40 0.50
8.56 10.65 13.12 16.35 19.42
6.59 7.44 8.59 9.69 11.30
4.62 5.26 6.15 6.97 7.88
0.4001/0.1501
0.10 0.20 0.30 0.40 0.50
10.85 13.41 17.50 23.58 30.19
7.12 8.65 11.26 14.47 17.77
5.16 6.14 7.63 9.38 12.50
1.72
3.69
Standard uncertainties u are u(T) = 0.1 K; u(w) = 0.0001; u(p) = 5 kPa; u(g) = 0.17 mPa s
T = 323.2 K
0.10 0.20 0.30 0.40 0.50
1.55
2.51
T = 313.2 K
0.3999/0.0501 TABLE 3 Viscosities of CO2-unloaded DEAE aqueous solutions. p = 0.1 MPa.
g/(mPa s)
g/(mPas) T = 303.2 K
i¼1
wDEAE
g/(mPa s) T = 303.2 K
ð7Þ
where gwater is the viscosity of pure water, and w ¼ w1 þ w2 is the total mass fraction of DEAE and MEA. The symbol f ða; wÞ refers to the contribution of CO2 loading:
fs ¼
Standard uncertainties u are u(T) = 0.1 K; u(w) = 0.0001; u(p) = 5 kPa; u(g) = 0.16 mPa s (g 5 10 mPa s); u(g) = 0.16 mPa s (10 mPa s < g).
Standard uncertainties u are u(T) = 0.1 K; u(w) = 0.0001; u(p) = 5 kPa; u(g) = 0.18 mPa s (g 5 10 mPa s); u(g) = 0.29 mPa s (10 mPa s < g); wDEAE and wMEA are the initial mass fractions in the CO2-unloaded solutions.
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10
η/( mPa⋅s)
η/( mPa⋅s)
10
10
η/( mPa⋅s)
η/( mPa⋅s)
10
1 290
300
310
320
330
1 290
T/K
1
T 290
300
300
310
320
330
T/K
310
320
330
1 290
T/K
300
310
320
330
T/K
FIGURE 2. Temperature dependence of the viscosity of CO2-unloaded DEAE–MEA aqueous solutions at wDEAE = 0.40 and wDEAE = 0.30 (insert plot). Symbols: experimental values from this work, j wMEA = 0.05; d wMEA = 0.10; ▲ wMEA = 0.15. Lines: calculated values.
FIGURE 4. Temperature dependence of the viscosity of CO2-loaded DEAE–MEA aqueous solutions at wDEAE/wMEA = 0.40/0.10 and wDEAE/wMEA = 0.30/0.10 (insert plot). Symbols: experimental values from this work, j a = 0.1; d a = 0.3; ▲ a = 0.5. Lines: calculated values.
find that the viscosity increases with the increase of wMEA at a given temperature and given wDEAE, and exponentially decreases with the increase of temperature at a given wDEAE and given wMEA. Figure 3 shows the CO2 loading dependence of the viscosity of CO2-loaded DEAE–MEA aqueous solutions, indicating that at a given temperature, given wDEAE and wMEA, the viscosities of carbonated aqueous solutions increase monotonously with the increase of CO2 loading. Figure 4 shows the temperature dependence of the viscosity of CO2-loaded aqueous solutions, indicating that at given CO2 loading, given wDEAE and wMEA, the viscosity exponentially decreases with increasing temperature. The Weiland equation correctly captures the temperature, mass fraction of amine and CO2 loading dependences of the viscosities and the calculated results match the experimental values satisfactorily.
η/( mPa⋅s)
10
η/( mPa⋅s)
10
4. Conclusions 1 0.0
0.2
0.4
0.6
0.8
α
1 0.0
0.2
0.4
0.6
0.8
In this work, the absorption of CO2 in MEA promoted DEAE aqueous solution was investigated at temperatures ranging from (303.2 to 323.2) K. The viscosities of both CO2-unloaded and CO2-loaded DEAE–MEA aqueous solutions were measured and calculated. Our results show that:
α FIGURE 3. CO2 loading dependence of the viscosity of CO2-loaded DEAE–MEA aqueous solutions at wDEAE/wMEA = 0.40/0.10 and wDEAE/wMEA = 0.30/0.10 (insert plot). Symbols: experimental values from this work, j T = 303.2 K; d T = 313.2 K; ▲ T = 323.2 K. Lines: calculated values.
where the superscripts ‘exp’ and ‘cal’ respectively stand for the experimental and calculated values, and n represents the number of data points. The optimized values are: a1 = 0.1838, b1 = 4.9811, c1 = 20.2088, d1 = 4342.9, e1 = 0.00317, f1 = 0.00256, g1 = 0.00929. The average relative deviation (ARD) is 4.14%. Figure 2 shows the values of viscosity of CO2-unloaded DEAE– MEA aqueous solutions calculated from the Weiland equation, and the comparison with experiments. From this figure, one may
(1) The solution viscosity affects the solubility of CO2. The increase of viscosity may sometimes lower the diffusion coefficient of the gas in the solution, hence leading to abnormalities in solubility. (2) For CO2-unloaded DEAE–MEA aqueous solution, the viscosity increases with the increase of the wMEA at a given temperature and wDEAE, and exponentially decreases with the increase of temperature at a given wMEA and wDEAE. (3) For CO2-loaded DEAE–MEA aqueous solution, the viscosity increases monotonously with the increase of CO2 loading and exponentially decreases with increasing temperature. (4) The Weiland equation can correctly capture the effects of CO2 loading, mass fraction of amines and temperature on viscosity, and satisfactorily fits the experimental values.
D. Fu et al. / J. Chem. Thermodynamics 95 (2016) 136–141
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JCT 15-581