Fluid Phase Equilibria 399 (2015) 4049

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Fluid Phase Equilibria

j o u r n a l h o m e p a g e : w w w . e l s e v i e r . c o m / l o c a t e / fl u i d

CO2 absorption into aqueous potassium salts of lysine and proline:

Density, viscosity and solubility of CO2
Shufeng Shen a,b, * , Ya-nan Yang a , Yong Wang a , Shaofeng Ren a,b , Jiangze Han a ,
Aibing Chen a
a
b

School of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China
Hebei Research Center of Pharmaceutical and Chemical Engineering, Shijiazhuang 050018, China

A R T I C L E I N F O

A B S T R A C T

Article history:
Received 13 February 2015
Received in revised form 15 April 2015
Accepted 24 April 2015
Available online 25 April 2015

Amino acid salts have potential use as alternative absorbents to alkanolamines for post combustion CO2
capture, because of their negligible volatility, resistance to oxidative degradation and fast absorption
rates. In this work, the density and viscosity of CO2-free and CO2-loaded aqueous solutions of potassium
lysinate (LysK) and potassium prolinate (ProK) were measured at temperatures from (298.15 to 348.15) K
and for their concentrations from (0.2 to 3.0) mol L
1. The data were correlated accurately (R2  0.99) as a
function of temperature, concentration and CO2 loading by nonlinear regression analysis. The solubility
of CO2 in 2.5 mol L
1 amino acid salt solutions was also determined in vaporliquid equilibrium vessels at
temperatures (313 and 333) K and CO2 partial pressures relevant to ue gas conditions. It was found that,
the CO2 absorption capacity of LysK is higher than that of industrially used monoethanolamine (MEA) and
the CO2 loadings vary as LysK > ProK > MEA at given CO2 partial pressures. Moreover, LysK may offer
higher cyclic loading than MEA for CO2 capture.
2015 Elsevier B.V. All rights reserved.

Keywords:
Density
Viscosity
CO2 solubility
Potassium lysinate
Potassium prolinate
Vaporliquid equilibrium

1. Introduction
One of the most disturbing global environmental problems is
global warming and climate change. This problem is most likely
caused by the increasing carbon dioxide (CO2) concentration in
atmosphere from a variety of emission sources such as the
combustion of fossil fuels (coal and natural gas) for power
generation, chemical industrial processes as well as human
activities. CO2 capture by chemical absorption remains the most
promising technology to reduce CO2 emissions. This technology
employs the chemical solvents which can reversibly react with
CO2. Amine-based solvents particularly monoethanolamine (MEA)
have been the most studied absorbents for this capture process
[13]. However, these solvents also exhibit several drawbacks such
as high energy consumption for regeneration, limited CO2 capacity,
thermal and oxidative degradation [4]. Improvements of energy
efciency and cost reduction are needed but these should at the

* Corresponding author at: Hebei University of Science and Technology, School of

Chemical and Pharmaceutical Engineering, No.70 Yuhua East Road, Shijiazhuang
050018, China. Tel.: +86 311 88632183; fax: +86 311 88632183.
E-mail addresses: sfshen@hebust.edu.cn, shufengshen@gmail.com (S. Shen).
http://dx.doi.org/10.1016/j.uid.2015.04.021
0378-3812/ 2015 Elsevier B.V. All rights reserved.

same time improve the environmental aspects of the process. One

solution to enhance process performance is to apply attractive
alternative absorbents such as amino acid based solvents and
promoted carbonate-based solvents [2,58]. Aqueous alkaline salts
of amino acid have received particular interest because many
amino acids are benign chemicals and have more favorable
properties such as low volatility (due to their ionic nature), low
toxicity, high level of biodegradability. They have the same
functional group like amines and can react with CO2 in a similar
way. Several potassium salts of amino acids such as glycine,
proline, taurine, alanine, threonine, sarcosine and arginine are
under extensive investigation on kinetics of absorption and have
been found good potential as solvents for CO2 capture [618].
Physicochemical properties of absorbents such as density,
viscosity and CO2 solubility are necessary for detailed characterization of the solvent for industrial application and they are
required in the process modeling, simulation and design of
gasliquid contactor columns for CO2 absorption and regeneration
[1921]. These data are also necessary to deduce chemical reaction
kinetics from CO2 absorption rate experiments. Kumar et al. [22,23]
and Wei et al. [24] reported the densities and viscosities of 0.46 M
potassium taurate and CO2 solubility in 26 M potassium taurate
solution over the temperature range of 293353 K. The properties

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

Nomenclature
AAD
AAS
C
ki
Ki
P
PCO2
P CO2
PH2 O T
R
wt%
T
yCO2 IR

Average absolute deviation, dimensionless

Amino acid salt
The molar concentration of the solution, (mol L
1)
The tting polynomial coefcients, dimensionless
The tting polynomial coefcients, dimensionless
Total pressure in the equilibrium vessel, (kPa)
CO2 partial pressure in gas bulk phase, (kPa)
Equilibrium partial pressure, (kPa)
The vapor pressure of water in the equilibrium vessel,
(kPa)
The gas constant, 8.3145, (m3 Pa K
1 mol
1)
Weight percentage, dimensionless
Absolute temperature, (K)
mol fraction of CO2 measured by gas analyzer,
dimensionless

Greek letters
a CO2 loading, the moles of CO2 per mol of absorbent (mol
CO2 /mol absorbent)
r The density, (g cm
3)
h The viscosity, (mPa s
1)

Table 1
Description of chemical samples used in this study.
Chemical
name

Molar
mass

Source

Purity
(mass
fraction)

Purication
method

L-Lysine

146.19
115.13
61.08
56.11

Aladdin Industrial Inc.

Aladdin Industrial Inc.
Tianjin Yongda reagent
Aladdin Industrial Inc.
(anhydrous)

98.0%
99.0%
99.0%
95.0%

None
None
None
None
Tianjin
Yongda
reagent

L-Proline

MEA
KOH
K2CO3

138.21
99.0%
H2SO4
NaOH
CO2

None
98.08
Standard
solution
44.01

N2

28.01

Density
standard
Standard
gas S1

Tianjin Yongda reagent

Tianjin Yongda reagent
Aladdin Industrial Inc.
Shijiazhuang Xisanjiao
oxygen generation
station
Shijiazhuang Xisanjiao
oxygen generation
station
Anton Paar GmbH,
Austria
Nanjing Special Gas
Factory Co., Ltd.

Standard
gas S2

Nanjing Special Gas

Factory Co., Ltd.

Water

of CO2-free and CO2-loaded taurate solution and 30% MEA were

also compared. Shaikh et al. [25] recently reported the properties
such as density, viscosity and refractive index of aqueous solutions
of sodium prolinate (SP) with 0.050.40 mass fractions at
temperatures from 298.15 K to 343.15 K. Majchrowicz et al. [26]
and Chang et al. [27] measured the solubility of CO2 in aqueous
potassium salt of L-proline solutions. A benecial effect of the
precipitation formation on the overall CO2 solubility was
discussed. Holst et al. [19] and Titona et al. [28] examined
physicochemical properties such as density, viscosity, refractive
index and electrical conductivities of aqueous alkali salts of alanine
at temperatures from (303.15 to 343.15) K and concentrations
ranging from (0.5 to 3.5) M. Aronu et al. [29] and Song et al. [30]
studied the physicochemical properties of aqueous potassium salts
of sarcosine and serine. To the best of our knowledge, the data of
such properties of potassium lysinate have not yet been reported in
the open literature. Moreover, the reported data for aqueous
potassium prolinate solutions are rare and scattered. Effect of CO2
loading on these properties is also unavailable. Therefore, in the
present work, we presented experimental data on density,
viscosity and CO2 solubility of CO2-free and CO2-loaded aqueous
potassium salts of lysine and proline. Measurements were made
for potassium lysinate concentrations from (0.2 to 3.0) M and
temperatures from (298.15 to 348.15) K and for potassium
prolinate concentrations from (0.5 to 3.0) M and temperatures
from (298.15 to 348.15) K. Correlations of experimental values as a
function of temperature, concentration and CO2 loading were also
developed, which can be useful in calculations for the kinetics and
the design of capture processes.

41

18.02

Merck-Millipore Aquelix
5

The amino acids, L-Lysine (Lys CAS No. 56-87-1, 98% purity) and
(Pro CAS No. 147-85-3, 99% purity), and potassium
hydroxide (KOH, CAS No. 1310-58-3, GR, 95% purity) were
purchased from Aladdin Industrial Inc., China. Sulfuric acid
(H2SO4, CAS No. 7664-93-9, 98% purity) was supplied from Tianjin

L-Proline

None
None

99.999%
(v/v)

None

Ultra pure
water
10.02%
CO2/
89.98% N2
19.98%
CO2/
80.02% N2
15 MV

None

None

None

None

RO-Elix

Yongda reagent, China. N2 (99.99%, v/v) and CO2 (99.995%, v/v)

were obtained commercially. Standard N2/CO2 mixed gases, S1
(10.02% CO2) and S2 (19.98% CO2) were purchased from Nanjing
Special Gas Factory Co., Ltd. and used for calibration of a CO2 gas
analyzer with a resolution of 0.01% (GXH-3011N, 0  20%, Institute

Table 2
Comparison of experimental data of density (r) and viscosity (h) of pure
compounds with literature values.a
T(K)

r (g cm
3)

h (mPa s
1)

This work

Ref. [32,33]

Water

293.15
298.15
303.15
308.15
313.15
318.15

0.9982
0.9971
0.9957
0.9940
0.9922
0.9902

0.99821
0.99704
0.99565
0.99403
0.99221
0.99021

MEA

303.15

1.0077

1.0098 [34]
1.0091 [36]
1.0084 [37]

14.6050

15.1058 [35]
15.1940 [36]
14.88 [37]

313.15

0.9998

1.0022 [34]
1.0013 [36]
1.0001 [37]

9.7244

10.0284 [35]
10.0283 [36]
9.93 [37]

323.15

0.9917

0.9944 [34]
0.9934 [36]
0.9919 [37]

6.8067

6.9715 [35]
6.9463 [36]
6.89 [37]

333.15

0.9837

0.9862 [34]
0.9854 [36]
0.9836 [37]

4.9695

5.0473 [35]
5.0454 [36]
4.97 [37]

343.15

0.9755

0.9774 [34]
0.9771 [36]

3.7838

3.7793 [35]
3.8050 [36]

2. Materials and methods

2.1. Materials and amino acid salt preparation

98.0%
0.5051 M
0.5000 N
99.995%
(v/v)

This work
1.0016
0.8908
0.7990
0.7220
0.6564
0.6009

Ref. [32,33]
1.0016
0.89002
0.79722
0.7230
0.65273
0.5990

a
Measurements were performed at 101.3  0.2 kPa. The measurement uncertainties u are u(T) = 0.02 K, u(r) = 0.0001 g cm
3,u(h) =  0. 5%.

42

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

[(Fig._1)TD$IG]

Fig. 1. A schematic diagram of experimental apparatus for vaporliquid equilibrium measurement.

electronic analytical balance (OHAUS, CP214) was used for weight

measurements with a precision of 0.1 mg. CO2-loaded amino acid
salt solutions were prepared by bubbling CO2 from a gas cylinder in
a ask. The exact concentrations of amino acid salt were
determined by potentiometric titration during vaporliquid
equilibrium experiments and CO2 loading (a) of solutions was
measured by the Chittick CO2 apparatus [31]. a is dened as the
moles of CO2 per mole of amino acid salt (AAS), mol CO2/mole AAS.

of Beijing HUAYUN Analytical Instrument). Titration was performed using an automatic potentiometric titrator (ZDJ-5, INESA
Scientic Instrument Co., Ltd.) with a precision of 0.1 mV. All the
reagents were used without further purication. A chemical
sample description is given in Table 1.
The aqueous amino acid salt solutions were prepared by
neutralizing the amino acid dissolved in deionized water with an
equimolar amount of KOH in a volumetric ask at 293 K  1.0 K. An

Table 3
Density of CO2-free and CO2-loaded aqueous potassium lysinate or prolinate solutions at 101.3  0.2 kPa.a
C (mol L
1)

ab

T (K)
298.15
r (g cm
3)

303.15

308.15

313.15

318.15

323.15

328.15

333.15

338.15

343.15

348.15

Potassium salt of lysine

0.2001
0
0.2500
0
0.5000
0
0.7500
0
1.0082
0
1.5291
0
1.7900
0
1.9999
0
2.5000
0
3.0000
0
2.5000
0.3466
0.4276
0.5091
0.6008
0.6999
0.7103
0.8760
1.0431
1.1089

1.0105
1.0175
1.0282
1.0432
1.0560
1.0848
1.1110
1.1216
1.1419
1.1510
1.1620
1.1692
1.1708
1.1816
1.1960
1.1958
1.2029
1.2130
1.2206

1.0090
1.0160
1.0271
1.0414
1.0541
1.0827
1.1086
1.1191
1.1391
1.1483
1.1594
1.1666
1.1682
1.1790
1.1934
1.1933
1.2004
1.2104
1.2180

1.0073
1.0142
1.0252
1.0395
1.0520
1.0804
1.1060
1.1165
1.1364
1.1455
1.1567
1.1641
1.1656
1.1765
1.1908
1.1908
1.1979
1.2067
1.2154

1.0054
1.0123
1.0232
1.0373
1.0498
1.0779
1.1034
1.1138
1.1335
1.1426
1.1540
1.1614
1.1630
1.1740
1.1882
1.1883
1.1954
1.2041
1.2127

1.0033
1.0102
1.0210
1.0351
1.0475
1.0754
1.1008
1.1110
1.1306
1.1397
1.1513
1.1587
1.1603
1.1713
1.1855
1.1857
1.1927
1.2013
1.2100

1.0011
1.0079
1.0186
1.0327
1.0450
1.0728
1.0981
1.1081
1.1276
1.1367
1.1486
1.1560
1.1577
1.1686
1.1828
1.1813
1.1899
1.1985
1.2072

0.9986
1.0054
1.0162
1.0301
1.0424
1.0701
1.0952
1.1052
1.1246
1.1337
1.1458
1.1532
1.1550
1.1658
1.1799
1.1787
1.1870
1.1956
1.2043

0.9956
1.0028
1.0137
1.0275
1.0397
1.0672
1.0923
1.1022
1.1215
1.1306
1.1429
1.1503
1.1523
1.1629
1.1770
1.1758
1.1841
1.1927
1.2014

0.9934
1.0028
1.0110
1.0247
1.0369
1.0643
1.0893
1.0991
1.1183
1.1275
1.1399
1.1473
1.1493
1.1599
1.1740
1.1728
1.1812
1.1898
1.1985

0.9906
0.9973
1.0081
1.0218
1.0339
1.0613
1.0863
1.0960
1.1150
1.1243
1.1368
1.1442
1.1462
1.1568
1.1710
1.1698
1.1782
1.1867
1.1954

0.9877
0.9943
1.0052
1.0187
1.0309
1.0582
1.0832
1.0927
1.1118
1.1211
1.1336
1.1411
1.1430
1.1537
1.1680
1.1667
1.1751
1.1837
1.1924

Potassium salt of proline

0.5001
0
1.0000
0
1.5000
0
2.0002
0
2.5000
0
3.0000
0
3.0000
0.0915
0.2725
0.5198
0.6399

1.0266
1.0547
1.0880
1.1114
1.1458
1.1669
1.1715
1.1974
1.2131
1.2218

1.0252
1.0530
1.0864
1.1092
1.1432
1.1641
1.1688
1.1947
1.2104
1.2191

1.0235
1.0510
1.0845
1.1070
1.1406
1.1613
1.1660
1.1919
1.2076
1.2163

1.0216
1.0490
1.0822
1.1047
1.1379
1.1584
1.1632
1.1891
1.2047
1.2135

1.0196
1.0468
1.0812
1.1025
1.1351
1.1555
1.1602
1.1862
1.2017
1.2106

1.0176
1.0445
1.0788
1.1004
1.1322
1.1525
1.1572
1.1832
1.1987
1.2076

1.0152
1.0422
1.0766
1.0985
1.1292
1.1494
1.1511
1.1802
1.1956
1.2046

1.0128
1.0399
1.0747
1.0958
1.1262
1.1463
1.1542
1.1771
1.1924
1.2015

1.0104
1.0374
1.0737
1.0936
1.1230
1.1431
1.1479
1.1739
1.1892
1.1983

1.0080
1.0355
1.0719
1.0943
1.1199
1.1398
1.1446
1.1707
1.1859
1.1950

1.0056
1.0357
1.0705
1.0924
1.1166
1.1365
1.1413
1.1643
1.1825
1.1917

a
b

The measurement uncertainties u are u(T) = 0.02 K, u(r) = 0.0001 g cm
3, u(a) = 0.002.
a is dened as the moles of CO2 per mole of amino acid salt (AAS), mol CO2 /mole AAS.

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

43

[(Fig._2)TD$IG]

2.2. Density measurement

1.15

Density measurements were performed using a digital

oscillating tube densimeter (Anton Paar, DMA-4100 M) having
stated precision of 1.0  10
4 g cm
3. It had an integrated
thermostat with Pt-100 thermometer and a low-thermal mass
measuring cell (a U-shaped borosilicate glass tube), which
enabled rapid changes and exact adjustments to the measuring
temperature. The temperature was controlled to 0.01 K of the
set value, and the precision of the measured value was 0.02 K.
The densimeter was calibrated using dry air and distilled
deionized water as standard uids. The calibration was
validated by measuring the water and pure MEA at the
measuring range considered in this work. The validated results
are given in Table 2.

0.2001 M
0.2500 M
0.5000 M
0.7500 M
1.0082 M
1.5291 M
1.7900 M
1.9999 M
2.5000 M

, g.cm

-3

1.10

1.05

1.00
290

2.3. Viscosity measurement

300

310

320

330

340

350

360

T, K

Viscosity measurements were done using a digital rolling

ball microviscometer (Anton Paar, Lovis 2000 M/ME) with the
precision up to 0.5%. The viscometer had a built-in Pt100 temperature sensor for temperature control of capillary
and measurement (uncertainty of 0.02 K). In the present work,
measurements were performed using a capillary with diameter
d = 1.59 mm, which allowed measurements for a wide range of
viscosities (0.390) mPa s
1. Before and after each measurement,
the viscometer was carefully calibrated with deionized water.
The calibration was validated by measuring the viscosity of the
density standard water and pure MEA, which the viscosity of our
samples is within the viscosity range in the investigated
temperature range. The results of the validation are also given
in Table 2. Six measurements were carried out to report the
viscosity data in average.

Fig. 2. Density of aqueous potassium lysinate solutions at different temperatures

and concentrations. Line: correlation results from Eq. (2).

[(Fig._3)TD$IG]

2.4. Vaporliquid equilibrium experiments

PCO2 P
PTH2 O yIR

CO2

(2)

where P and PTH2 O are the total pressure in the vessel and the vapor
pressure of water in the equilibrium vessel at the equilibrium
temperature, respectively. yIR
CO2 is mol fraction of CO2 measured by
gas analyzer with drying tube.

Fig. 3. Effect of CO2 loading on density of 2.5 M aqueous potassium lysinate

solutions at various temperatures. Line: correlation results from Eq. (3).

[(Fig._4)TD$IG]
1.20
0.5001 M
1.0000 M
1.5000 M
2.0002 M
2.5000 M
3.0000 M

-3

1.15

1.10

, g.cm

CO2 absorption capacity in aqueous solutions of different

absorbents was determined in an absorption apparatus as
described in our previous work [5]. CO2 was bubbled through
the solutions at an operating temperature of 293 K until the CO2
loading became constant or precipitation occurred. The absorption
time to reach the points for these absorbents was various. The CO2
absorption capacity expressed in Kg CO2 per liter solvent was
obtained.
Vaporliquid equilibrium for amino acid salt solutions with
known CO2 loading was measured from 313 K to 343 K and at
near atmospheric pressure. A schematic diagram of the
experimental set-up was shown in Fig. 1. Absorbent samples,
120 cm3 each, were placed in three successive vessels submerged in a thermally regulated water bath (0.1 K). N2 was
rst ushed through the devices to purge out the gases within
the system, and then the gas phase was circulated and analyzed
online until steady values of CO2 concentration were recorded
by the online GXH-3011N gas analyzer. Total pressure in the
vessel was measured using pressure transducer with a full scale
uncertainty of 0.27 kPa (PX409-050AUSBH, 0  3.4 bar, Omega
Engineering Inc.). Equilibrium partial pressures of CO2, PCO2 , in
gas phase were calculated as follows:

1.05

1.00
290

300

310

320

330

340

350

360

T, K
Fig. 4. Density of aqueous potassium prolinate solutions at different temperatures
and concentrations. Line: correlation results from Eq. (2).

44

[(Fig._5)TD$IG]

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

AAD

n
yexp
ylit
1X
j i lit i j  100%
n i1
yi

(1)

where n is the number of experimental points and

yexp
andylit
i represent the experimental and literature values. It
i
was found from Table 2 that the measured data were in good
agreement with the data in the literature and the average absolute
deviation values are 0.0150.108% for density and 0.6471.064% for
viscosity, respectively. The deviation could be probably due to the
difference in purity and source of chemicals.
3.1. Density

Fig. 5. Effect of CO2 loading on density of 3.0 M aqueous potassium prolinate

solutions at various temperatures. Line: correlation results from Eq. (3).

3. Results and discussion

To validate the experimental methods and results, experimental measurement of density and viscosity of water standard and
pure MEA were measured at temperatures ranging from 293.15 K
to 343.15 K and compared with values from published work in
Table 2. The validity was evaluated by the average absolute
deviation (AAD) between experimental and published values.

The measured density results for aqueous solutions of

potassium lysinate and potassium prolinate at concentrations
up to 3.0 M and temperatures from (298.15 to 348.15) K are
presented in Table 3. The effect of temperature and CO2 loading
on density are shown in Figs. 25. It can be found that, with
increasing the concentration of amino acid salt in the solution,
the density increases; with increasing the CO2 loading, the
density increases greatly; however, the density decreases with
the rise of temperature for two amino acid salt solutions at a
given concentration and CO2 loading.
An additional goal of this work is to t suitable correlations for
physical properties (as a function of temperature, concentration
and/or CO2 loading), which could be applied to calculate their
properties in kinetic study and process simulation on CO2 capture.
The experimental densities were correlated to a polynomial
function that is temperature, concentration and/or CO2 loading
dependent, according to Eqs. (2) and (3), respectively.

Table 4
Viscosity of CO2-free and CO2-loaded aqueous potassium lysinate or prolinate solutions at 101.3  0.2 kPa.a
C (mol L)
1

ab

T (K)
298.15
303.15
h (mPa s
1)

308.15

313.15

318.15

323.15

328.15

333.15

338.15

343.15

348.15

Potassium salt of lysine

0.2001
0
0.2500
0
0.5000
0
0.7500
0
1.0082
0
1.5291
0
1.7900
0
1.9999
0
2.5000
0
3.0000
0
2.5000
0.3466
0.4276
0.5091
0.6008
0.6999
0.7103
0.8760
1.0431
1.1089

1.0031
1.0079
1.2899
1.3479
1.5747
2.2856
3.2362
3.5636
5.4062
8.4071
6.2327
6.8486
6.6842
7.7466
8.9513
8.6686
8.8287
9.3274
9.7656

0.8978
0.9023
1.1581
1.1996
1.3969
2.0071
2.8050
3.0545
4.5967
7.0267
5.3107
5.8179
5.7203
6.5530
7.6101
7.4006
7.5606
7.9124
8.2537

0.8095
0.8125
1.0454
1.0745
1.2473
1.7745
2.4540
2.6762
3.9504
5.9463
4.5779
5.0005
4.9261
5.6141
6.5429
6.3762
6.5201
6.9613
7.0592

0.7344
0.7377
0.9512
0.9697
1.1214
1.5815
2.1732
2.3578
3.4328
5.0939
3.9852
4.3377
4.2971
4.8710
5.6988
5.5291
5.6532
6.0767
6.1033

0.6711
0.6737
0.8660
0.8813
1.0138
1.4184
1.9344
2.1164
3.0085
4.4075
3.5015
3.8009
3.7787
4.2625
4.9789
4.8646
4.9671
5.3010
5.3343

0.6168
0.6185
0.7960
0.8040
0.9223
1.2798
1.7354
1.9159
2.6594
3.8517
3.0939
3.3574
3.3361
3.7546
4.3755
3.9953
4.3690
4.6739
4.6952

0.5697
0.5705
0.7351
0.7388
0.8431
1.1621
1.5660
1.7567
2.3683
3.3936
2.7595
2.9864
2.9879
3.3372
3.8796
3.5802
3.8970
4.1409
4.1611

0.5292
0.5294
0.6833
0.6798
0.7748
1.0606
1.4211
1.6208
2.1358
3.0120
2.4755
2.6763
2.6957
2.9864
3.4619
3.2248
3.4684
3.7020
3.7203

0.4937
0.4939
0.6409
0.6290
0.7155
0.9729
1.2960
1.5011
1.9272
2.6926
2.2358
2.4098
2.4351
2.6872
3.1042
2.9042
3.1194
3.3311
3.3438

0.4633
0.4630
0.6042
0.5855
0.6637
0.8961
1.1884
1.4351
1.7485
2.4232
2.0437
2.1815
2.2177
2.4458
2.8051
2.6378
2.8214
2.9941
3.0155

0.4359
0.4358
0.5715
0.5472
0.6181
0.8306
1.0945
1.3458
1.5943
2.2079
1.8602
2.0120
2.0422
2.2379
2.5512
2.4064
2.5622
2.7137
2.7379

Potassium salt of proline

0.5001
0
1.0000
0
1.5000
0
2.0002
0
2.5000
0
3.0000
0
3.0000
0.0915
0.2725
0.5198
0.6399

1.1047
1.3800
1.8613
2.2927
3.1809
4.0539
4.1610
4.8399
4.9079
5.1655

0.9857
1.2318
1.6423
2.0282
2.7552
3.4909
3.5826
4.1514
4.2133
4.4409

0.8913
1.1032
1.4652
1.7944
2.4092
3.0383
3.1140
3.5984
3.6591
3.8558

0.8086
0.9949
1.3105
1.6012
2.1360
2.6618
2.7313
3.1510
3.2061
3.3802

0.7351
0.9035
1.2000
1.4391
1.9028
2.3539
2.4155
2.7833
2.8350
2.9899

0.6741
0.8251
1.0847
1.2961
1.7068
2.1018
2.1633
2.4770
2.5254
2.6630

0.6219
0.7569
0.9922
1.1957
1.5415
1.8866
1.7549
2.2179
2.2646
2.3899

0.5764
0.7002
0.9175
1.0930
1.4001
1.7041
1.9424
2.0110
2.0573
2.1575

0.5373
0.6493
0.8552
1.0086
1.2781
1.5493
1.5946
1.8236
1.8685
1.9663

0.5039
0.6080
0.7966
0.9587
1.1731
1.4140
1.4562
1.6629
1.7065
1.7958

0.4733
0.5792
0.7486
0.8972
1.0818
1.2993
1.3370
1.4668
1.5666
1.6473

a
b

The measurement uncertainties u are u(T) =  0.02 K, u(a) = 0.002, u(h) = 0.5%.
a is dened as the moles of CO2 per mole of amino acid salt (AAS), mol CO2/mole AAS.

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

45

Table 5
Fitting parameters of Eq. (2) a and (3) b for density of aqueous potassium salt solution of amino acids.
R2

AADc (%)

0.06789

0.9929
0.9971

0.287
0.270

0.08356

0.9943
0.9960

0.269
0.283

Amino acid

No. of data points

CO2 loaded solution data included

ki (i = 0, 1, 2); Ki (i = 0, 1, 2, 3)
0

Lysine

99
187

NO
YES

1.15704
1.16568

5.16283  10
4

5.39647  10
4

0.05652
0.05501

Proline

66
110

NO
YES

1.14167
1.16121

4.64606  10
4

5.22855  10
4

0.05486
0.05425

a
b
c

r k0 k1 T k2 C.
r K 0 K 1 T K 2 C K 3 a.

n
X
rexp
rcalc
AAD 1n j i rexp i j.
i1

r k0 k1 T k2 C

(2)

r K0 K1T K2C K3a

(3)

where r is the density in g cm3; T is the absolute temperature in K;

C is the molar concentration of the solution in mol L
1 (M); a is the
CO2 loading of the solution, mol CO2/mole AAS; ki (i = 0 to 2) and Ki
(i = 0 to 3) are the polynomial coefcients obtained by tting the
equations to the experimental data by the nonlinear least squares
regression. The optimized coefcients were determined by
minimizing the objective function r in term of the AAD, which
are presented in Table 5. The values of R2 of both equations are
above 0.99 and the maximum AAD for both amino acid salts is
lower than 0.29%. The curved lines in Figs. 25 correspond to the
calculated values from Eq. (2) or (3). As shown, the lines from
Eq. (2) are in fairly good agreement with the experimental data
especially for potassium prolinate and potassium lysinate in a low
concentration range.
3.2. Viscosity
The measured viscosity results for aqueous solutions of
potassium lysinate and potassium prolinate at different concentrations and temperatures are given in Table 4, and the viscosity
versus temperature, concentration and CO2 loading is shown in
Figs. 69.
As known, the viscosity of absorbents can affect the CO2
absorption rate. Solvents with low viscosity can increase the

[(Fig._6)TD$IG]
[(Fig._7)TD$IG]

6.00
0.2001 M
0.2500 M
0.5000 M
0.7500 M
1.0082 M
1.5291 M
1.7900 M
1.9999 M
2.5000 M

5.00

4.00
, mPa.s

diffusion coefcient of CO2 in the liquid phase, which results in low

mass transfer resistance. As can be seen that for both systems, the
viscosity decreases with an increase in temperature at all
concentrations studied. However, with increasing the concentration of absorbents, the viscosity tends to increase. The similar
trends of variation in viscosity with concentration and temperature are found for other amino acid salts in the reported work
[25,2830]. After analysis of the experimental data, it was found
that the viscosities of lysinate solutions are higher than those of
prolinate solutions at same conditions. The viscosities of both
amino acid salt solutions increase after loading with CO2. The more
CO2 absorbed, the more viscous the solutions. The effect of
temperature on viscosity of both absorbents at high concentrations
from (1.5 to 3.0) M is greater than that at concentrations blew
1.0 M. For example, the viscosity of 2.5 M potassium lysinate
decreases from 5.40 cP at 298.15 K to 2.37 cP at 328.15 K. but for
0.5 M potassium lysinate, it decreases from (1.29 to 0.73) cP in the
same temperature range. It is also noted that the viscosities of
1.5 M lysinate solutions and 2.0 M prolinate solutions are similar to
the commonly used 30% MEA (4.97 M) at temperatures of 298
343 K. This indicates the diffusion coefcients of CO2 in the highly
concentrated solutions will be lower than or similar to those in 30%
MEA solution.
Based on the common description that the effect of temperature on viscosity of uids can be expressed by the Arrhenius
relationship, two temperature-, concentration- and/or CO2 loading- dependent exponential-type equations are correlated to Eqs.
(4) and (5) by tting the experimental data.

3.00

2.00

1.00

0.00
290

300

310

320

330

340

350

T, K
Fig. 6. Viscosity of aqueous potassium lysinate solutions at different temperatures
and concentrations. Line: correlation results from Eq. (4).

Fig. 7. Effect of CO2 loading on viscosity of 2.5 M aqueous potassium lysinate

solutions at various temperatures. Line: correlation results from Eq. (5).

46

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

[(Fig._8)TD$IG]

concentration; T is the absolute temperature in K; R is the gas

constant, 8.3145 m3 Pa K
1 mol
1; C is the molar concentration of
the solution in mol L
1; a is the CO2 loading of the solution, mol
CO2 / mole AAS; ki (i = 0 to 3) and Ki (i = 0 to 4) are the tting
coefcients by the nonlinear regression. The optimized coefcients
are listed in Table 6. The calculated values from Eq. (4) or (5) are
also presented as curved lines in Fig. 69. The values of R2 (0.99)
of tting Eqs. (4) and (5) and the maximum AAD between
experimental and the predicted data are in good agreement with
each other. Hence, the proposed correlations along with the
parameters could be used to obtain reliable prediction of the
viscosities of the aqueous amino acid salt solutions investigated in
the range of concentrations and temperatures in the present work.

5.00
0.5001 M
1.0000 M
1.5000 M
1.9999 M
2.5000 M
3.0000 M

4.00

, mPa.s

3.00

2.00

1.00

3.3. CO2 solubility

0.00
290

300

310

320

330

340

350

T, K
Fig. 8. Viscosity of aqueous potassium prolinate solutions at different temperatures
and concentrations. Line: correlation results from Eq. (4).

[(Fig._9)TD$IG]

3.3.1. Validation of experimental method

To validate the experimental method used in this work, a series
of experiments on CO2 solubility in 30 wt% (4.97 M) MEA solution
at T = 313.2 K and 35 wt% potassium carbonate (K2CO3) at
T = 343.2 K were performed. Before entering the CO2 gas analyzer,
the gas stream is required to cool down to eliminate the effect of
water vapor. Values of 7.36, 19.95 and 31.25 kPa were used for PTH2 O
over absorbent solutions at 313, 333 and 343 K respectively.
Variation of these values are neglected at the investigated loadings.
The vaporliquid equilibrium results are listed in Table 7. These
results from the present work are also presented in Fig. 10
alongside those reported from Endo et al. [38], the default ASPEN
plus E-NRTL values [39] and Aronu et al. [40]. A reasonable
agreement can be observed for both systems in the temperature
range investigated. Therefore, the method and apparatus used are
reasonable and reliable.

Fig. 9. Effect of CO2 loading on viscosity of 3.0 M aqueous potassium prolinate

solutions at various temperatures. Line: correlation results from Eq. (5).

h k0 exp



k1 expk2 C
expk3 C
RT

(4)



K 1 expK 2 C
expK 3 CexpK 4 a
RT

(5)

h K 0 exp

where h is the viscosity in mPa s; the activation energy of ow (Ea)

is described by an exponential-type relation dependent on the

3.3.2. CO2 solubility in aqueous solutions of potassium lysinate and

potassium prolinate
Comparison of CO2 absorption capacity in the 2.5 M amino acid
salt systems studied at 293 K with 30 wt% MEA solution (4.97 M) is
shown in Fig. 11. The maximum absorption capacity by MEA
solvent is approximately 0.114 Kg CO2/L, which is similar to the
reported (0.360.38 Kg CO2 per Kg MEA) [4143]. The absorption
capacity in 2.5 M LysK and 2.5 M ProK is 0.129 and 0.09 Kg CO2/L,
respectively. Potassium lysinate presents a higher absorption
capacity at the same solution concentration. The maximum CO2
loading in 2.5 M LysK and 2.5 M ProK is 1.20 and 0.81 mol CO2/mol
AAS, respectively. Hence, LysK was found superior compared to the
two others on the basis of absorption capacity. It could be a
promising alterative to alkanolamine absorbents (say, MEA).
Equilibrium CO2 solubility in aqueous solutions of 2.5 M LysK
and 2.5 M ProK at 313 and 333 K are given in Table 8. In the present
work, the experimental VLE data will be focused on situations
where no precipitation occurred. The measurements were

Table 6
Fitting parameters of Eq. (4) a and (5)b for viscosity of aqueous potassium salt solution of amino acids.
R2

AADc (%)

0.53089

0.9912
0.9947

5.23
4.52

0.34943

0.9964
0.9948

2.89
3.20

Amino acid

No. of data points

CO2 loaded solution data included

ki (i = 0, 1, 2, 3); Ki (i = 0, 1, 2, 3, 4)
0

Lysine

99
187

NO
YES

1.140  10
3
8.889  10
4

16445.8
17144.5

0.09225
0.09753

0.03955

0.04627

Proline

66
110

NO
YES

1.710  10
3
1.790  10
3

15558.2
15481.4

0.07385
0.08667

0.02585

0.12272

2 C
h k0 expk1 expk
expk3 C.
RT

2 C
h K 0 expK 1 expK
expK 3 CexpK 4 a.
RT

n
X
hexp
hcalc
AAD 1n j i hexp i j.
i1

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

47

Table 7
Solubility of CO2 in aqueous solutions of 4.97 M MEA and 35 wt% potassium carbonate at 313 and 343 K.a
35 wt% potassium carbonate

30 wt% MEA (4.97 M)

a (mol CO2/mole potassium ion)

PCO2*

0.114
0.145
0.192
0.234
0.287
0.330

0.160
0.270
0.535
0.970
1.977
2.506

a (mol CO2/mole AAS)

PCO2* (kPa) at 343 K

0.518
0.505
0.492
0.493
0.490
0.491
0.488
0.475
0.473
0.423
0.409

13.940
11.631
7.621
5.377
4.314
4.199
3.594
2.572
1.992
0.380
0.313

The measurement uncertainties u are u(T) = 0.1 K, u(a) = 0.002, u(PCO2*) = 0.02 kPa.
PCO2*: equilibrium partial pressure of CO2.

performed in the range of partial pressures of CO2 varying between

0.05 and 17.5 kPa, which is the range typically encountered in CO2
removal from ue gas at fossil fuel red power generation. Fig. 12
also presents the VLE results for the two amino acid salt systems
along with those for 30 wt% MEA solution, which is one of the most
widely used CO2 absorbents nowadays.
It can be observed that the CO2 partial pressures increase with
increasing the CO2 loading for all absorbents investigated. For a
given absorbent and CO2 partial pressure, the CO2 loading tends to
decrease as temperature increases. The results suggest that the CO2
solubility decreases with increasing temperature. Similar trends
can also be found for other amino acid salts: glycinate and taurate
[21,24]. This behavior can be attributed to the exothermic nature of
CO2 absorption.
The CO2 loading ranges of three absorbents showed quite
different in the range of CO2 partial pressure between 0.1 and
10 kPa. At the CO2 partial pressure of 10 kPa and 313 K, which is the
most used operating conditions in the CO2 capture industrial
processes using amines, the equilibrium loadings can reach 0.5 for
MEA, 0.7 for ProK and 1.0 for LysK. From the relative positions of
equilibrium curves, absorption capacity is the highest for 2.5 M
LysK and the lowest for 30 wt% MEA. Of the two amino acid salts,
LysK has smaller slope of equilibrium curves than ProK, which may
offer higher cyclic loading for CO2 capture. It should also be noted

that, the equilibrium CO2 partial pressures are no more than 0.1 kPa
for 2.5 M LysK in the loading range of 0.20.6. These benet for
driving force PCO2
PCO2 and are the favorite features of a
promising absorbent for CO2 removal from ue gas streams.
Different equilibrium curves for these absorbents could be
attributed to their structures and solution pH. Two amino acid salts
having a-amino functional group can react with CO2 in the similar

[(Fig._1)TD$IG]
(a)

CO2 absorption capacity (Kg/L)

(kPa) at 313 K

T = 293K

0.12

0.09

0.06

[(Fig._10)TD$IG]

4.97M MEA

2.5M LysK

2.5M ProK

Absorbents

1.2

2.5M LysK
2.5M ProK

, molCO2/mol AAS

1.0

0.8

0.6

(b)
T= 293K

0.4
0.0
Fig. 10. Comparison of experimental and literature data of CO2 equilibrium partial
pressure over 35 wt% equivalent K2CO3 solution at 343 K and 30 wt% MEA at 313 K.
PC30 and PC35 represent 30 wt% and 35 wt% equivalent K2CO3 solution,
respectively. Default ASPEN: VLE data from default ASPEN plus E-NRTL model.

1.0

2.0

3.0
4.0
5.0
Elapsed absorption time, h

6.0

7.0

Fig. 11. CO2 absorption capacity of absorbents (a) and CO2 loading variation in 2.5 M
aqueous solution of potassium lysinate and potassium prolinate with the elapsed
absorption time (b) at 293 K and atmospheric pressure.

48

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

Table 8
Equilibrium solubility of CO2 in aqueous solutions of 2.5 M potassium lysinate and 2.5 M potassium prolinate at 313 and 333 K.a
Equilibrium partial pressure of CO2, PCO2* (kPa)

a (mol CO2/mole AAS)

313 K

a (mol CO2/mole AAS)

333 K

2.5 M Potassium lysinate

1.024
0.998
0.995
1.001
0.996
0.991
0.966
0.955
0.932
0.925
0.906
0.828
0.818
0.803

17.444
14.235
12.354
10.082
8.770
6.657
4.962
3.353
2.412
2.156
1.169
0.209
0.152
0.104

0.936
0.873
0.865
0.830
0.815
0.754
0.703
0.710
0.675
0.676
0.646
0.618

16.088
3.359
2.121
1.807
0.812
0.433
0.320
0.254
0.182
0.140
0.108
0.069

2.5 M Potassium prolinate

0.674
0.608
0.571
0.559
0.534
0.522
0.478

6.954
2.341
1.203
0.649
0.320
0.180
0.107

0.594
0.589
0.585
0.557
0.547
0.512
0.486
0.485
0.448
0.386
0.373

15.728
9.930
7.006
5.015
3.985
1.950
1.259
0.493
0.247
0.065
0.037

The measurement uncertainties u are u(T) = 0.1 K, u(a) = 0.002, u(PCO2*) = 0.02 kPa. Measurements were performed at 103.3  2.0 kPa.

[(Fig._12)TD$IG]

central role [45,46]. 2.5 M LysK has a pH of 10.011.8 in the loading

range investigated whereas a pH of 9.0-10.6 for 2.5 M ProK.
Solution of LysK is more basic than ProK at a specic loading.
Meanwhile, the stability of carbamates decrease with decreasing
basicity of a-amino group [22]. Therefore, the higher CO2 loading
for LysK can be observed. However, for MEA and ProK, only one
amino group is involved in the reaction. Two molecules are
required: one acting as a base accepting a proton and the other
forming a carbamate. Thus, the lower loadings are expected at a
given CO2 partial pressure.
4. Conclusions

Fig. 12. CO2 equilibrium partial pressures over 2.5 M amino acid salt solutions and
30 wt% MEA at 313 K and 333 K.

way as amines [2,68]. The amino group in ProK is involved in two

carbonnitrogen bond, so it is a secondary amino group. It is
expected that the carbamate can be formed in these solutions
during CO2 absorption. Lysinate also contains a basic aliphatic
e-amino group in its side chain with pKa 10.53 [44], which will be
positively charged with the increasing CO2 loading. The positive
charge may participate in hydrogen bond to associate with water,
which would be favorable for deprotonation from the CO2-amino
acid complex and facilitate the carbamate formation. Moreover,
the deprotonated e-amino group can react with CO2 as a primary
amino group in the low CO2 loading range where pH above 11.0.
Carbamate may undergo hydrolysis to bicarbonate and deprotonated amino group if the pH is suitable where OH
ion might play a

Aqueous solution of potassium lysinate (LysK) was proposed as

a novel candidate absorbent for CO2 absorption. Physicochemical
properties of aqueous solutions of LysK and ProK were measured at
temperatures from (298.15 to 348.15) K and for their concentrations from (0.2 to 3.0) mol L
1. Experimental results were
correlated well with empirical correlations including the parameters such as temperature, concentration and CO2 loading. The
solubility of CO2 in 2.5 mol L
1 amino acid salt solutions was
measured at temperatures (313 and 333) K and CO2 partial
pressures from (0.1 to 17.5) kPa. LysK has higher CO2 absorption
capacity than monoethanolamine (MEA) and has high cyclic
loading for CO2 capture. The CO2 loadings vary as LysK > ProK >
MEA at given CO2 partial pressures. In summary, our results have
demonstrated that 2.5 M LysK are superior to the widely used
30 wt% MEA in CO2 solubility and absorption.
Acknowledgements
The authors would like to acknowledge National Natural
Science Foundation of China (No.21206029), Hebei Provincial
Natural Science Foundation for Distinguished Young Scholars of
China (No.B2015208067), Hebei Provincial Natural Science Foundation of China (No.2012208022) and Hebei Provincial Scientic

S. Shen et al. / Fluid Phase Equilibria 399 (2015) 4049

Research Foundation for the Returned Overseas Chinese Scholars

(2013-2015) for nancial support and thank Minjie Zhang and Yun
Li for assistance in this study.
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