Measurement and Prediction of the Solubility of CO2 in Ester Mixture

doi:10.4236/lce.2011.21005

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Low Carbon Economy, 2011, 2, 26-31

doi:10.4236/lce.2011.21005 Published Online March 2011 (http://www.SciRP.org/journal/lce)

Measurement and Prediction of the Solubility of

CO2 in Ester Mixture

Xia Gui, Zhigang Tang, Weiyang Fei

State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing, China.

Email: [email protected]

Received October 4th, 2010; revised December 23rd, 2010; accepted December 29th, 2010.

ABSTRACT

The solubility of CO2 in ester mixtures under high pressures are studied in this article. The constant-volume method is

used to determine the solubility of CO2 in DMC + diethyl carbonate system, DMC + propyl acetate system, DMC +

propylene carbonate system, and DMC + ethylene carbonate system from 282.0 K to 303.0 K. It is found that the solu-

bility of CO2 in four mixed solvents follows the Henry’s law and the linear compound has a greater ability to dissolve

CO2 than the cyclic compound at the same temperature. Furthermore, a modified equation is proposed to fit the solu-

tion data and a better equation is obtained in this paper. This will be useful for the future research in the screening of a

potential physical solvent for CO2 capture.

Keywords: CO2 Solubility, Eter Mxture, Solubility Prediction

1. Introduction

There are several ways to separate and capture CO2 from

fossil fueled power plant which can be classified into

three general categories: pre-combustion capture, post-

ombustion capture and oxyfuel strategy. [1] The selec-

tion of a technology for a given capture route depends on

the features of the gas treated. Based on the method used

for CO2 removal, separating methods can be broadly

classified as solvent absorption, adsorption, membrane

and cryogenic fractionation. [2] Compared with other

methods, solvent absorption process, especially physical

solvent, tends to be a favored choice when the partial

pressure of CO2 is high. In addition, physical solvent can

be stripped by reducing operation pressure with little

heat.

Methanol, [3-6] propylene carbonate [7,8] and poly-

ethylene glycol dimethyl ether [9,10] are commonly used

physical solvent in CO2 capture process. A general trend

in CO2 capture research is to develop a new solvent that

has the potential for dramatic cost reduction. Dimethyl

carbonate (DMC), a “green” absorbent, with advantages

of high CO2 loading, has been proved to be an effective

and low cost absorbent for CO2 capture. [11] But the

characteristics of low boiling point and high freezing

point limit its application in industry. According to the

colligative properties of solutions, adding a non volatile

solute, can increase the boiling point and decrease the

freezing point of a solvent, which means a decreasing

loss of the solvent and an enlargement application range

respectively in CO2 capture process. Base on the above,

the absorption capacity of DMC combined with other

additive is studied in this paper.

2. Experiment Materials

CO2 with a volume fraction of 0.9999 was supplied by

BeiWen Gas in Beijing. DMC (C3H6O3, with a mass frac-

tion of 0.999, made in China), propylene carbonate

(C4H6O3, with a mass fraction of 0.999, made in China),

ethylene carbonate (C3H4O3, with a mass fraction of 0.999,

made in China), diethyl carbonate (C5H10O3, with a mass

fraction of 0.999, made in China), propyl acetate (C5H12O2,

with a mass fraction of 0.999, made in China) were all

obtained from Aladdin-Reagent Company in Shanghai. All

components were used without further purification. The

apparatus, experimental procedure and data processing

were described in detail by Xia Gui. [11] Four mixed sol-

vent (DMC + ethylene carbonate, DMC + propyl acetate,

DMC + diethyl carbonate, DMC + propylene carbonate)

were prepared, in which the amount of DMC is 50% by

volume in order to reduce errors in the measurement.

3. Pure Compound Properties

Experimental results for the phase equilibrium of CO2 in

DMC at high pressure are given as bellow. The molecu-

Measurement and Prediction of the Solubility of CO in Ester Mixture27

lar formula, Hildebrand parameter (Mpa1/2), and dielec-

tric constant for the five pure solvents are provided in

Table 1 [12-14].

4. Results and Discussions

The temperature T, the CO2 partial pressure p at the equi-

librium state, CO2 mole fraction xi in liquid-phase and the

estimated uncertainties ui, for the ternary systems CO2 +

DMC + propylene carbonate, CO2 + DMC + ethylene

carbonate, CO2 + DMC + diethyl carbonate and CO2 +

DMC + propyl acetate are presented in Table 2, Table 3,

Table 4, Table 5 and plotted in Figure 1, Figure 2,

Figure 3 and Figure 4.

Table 1. Hildebrand parameter (Mpa1/2) and dielectric con-

stant for DMC, propylene carbonate, ethylene carbonate,

diethyl carbonate and propyl acetate.

compound molecular

formula

Hildebrand

parameter/Mpa1/2 dielectric

constant

DMC C3H6O3 20.2 3.1

propylene

carbonate C4H6O3 27.2 64.4

ethylene

carbonate C3H4O3 30.1 89.6

diethyl carbonate C5H10O3 18 2.8

propyl acetate C5H12O2 17.8 5.6

Table 2. Mole fraction (xi), equilibrium pressure (p), and

uncertainties (ui) of CO2 in DMC + propylene carbonate

from 282.81 K to 313.75 K.

p/MPa xi u

i p/MPa xi u

T = 282.81 K

0.2592 0.0549 0.0009 1.5513 0.2879 0.0021

0.4156 0.0860 0.0021 1.6656 0.3106 0.0027

0.7905 0.1512 0.0017 1.8961 0.3465 0.0016

1.0601 0.1981 0.0027 2.0455 0.3735 0.0032

1.3298 0.2502 0.0028 2.2550 0.4068 0.0028

T = 298.69 K

0.3311 0.0423 0.0009 1.8901 0.2415 0.0024

0.5826 0.0744 0.0018 2.2296 0.2849 0.0014

0.9543 0.1219 0.0017 2.4782 0.3166 0.0012

1.3130 0.1677 0.0025 2.7687 0.3537 0.0017

1.6656 0.2127 0.0021 3.1073 0.3971 0.0023

T = 313.75 K

0.3669 0.0362 0.0008 2.7123 0.2678 0.0024

0.8047 0.0795 0.0018 3.4600 0.3416 0.0019

1.0921 0.1078 0.0017 3.8245 0.3776 0.0021

1.5709 0.1551 0.0020 4.2680 0.4214 0.0023

2.2200 0.2191 0.0012

Table 3. Mole fraction (xi), equilibrium pressure (p), and

uncertainties (ui) of CO2 in DMC + ethylene carbonate from

282.83 K to 313.67 K.

p/MPa xi u

i p/MPa xi u

T = 282.83 K

0.18840.0317 0.0010 1.2136 0.1980 0.0012

0.37720.0709 0.0016 1.3791 0.2246 0.0019

0.55570.0987 0.0022 1.5516 0.2508 0.0017

0.72220.1233 0.0016 1.7863 0.2854 0.0016

0.99900.1680 0.0023 1.9778 0.3142 0.0023

T = 298.78 K

0.17240.0179 0.0008 1.9874 0.2067 0.0017

0.42690.0444 0.0016 2.3351 0.2430 0.0021

0.80380.0836 0.0022 2.5806 0.2685 0.0019

1.06430.1107 0.0016 2.7079 0.2818 0.0023

1.36200.1417 0.0012 3.0797 0.3204 0.0019

1.70890.1778 0.0017

T = 313.67 K

0.29740.0231 0.0008 1.610 0.1243 0.0013

0.47980.0371 0.0017 2.1497 0.1661 0.0021

0.80230.0621 0.0017 2.5945 0.2004 0.0023

1.09390.0845 0.0024 3.2326 0.2496 0.0023

1.32830.1026 0.0013 3.6383 0.2811 0.0018

Table 4. Mole fraction (xi), equilibrium pressure (p), and

uncertainties (ui) of CO2 in DMC + diethy carbonate from

282.89 K to 313.58 K.

p/MPa xi u

i p/MPa xi u

T = 282.89 K

0.23410.0596 0.0012 1.45 0.3589 0.0022

0.51990.1367 0.0015 1.57 0.3876 0.0017

0.81110.2060 0.0020 1.7 0.4115 0.0019

1.02010.2553 0.0014 1.85 0.4444 0.0017

1.22170.3051 0.0014 2.03 0.4902 0.0022

T = 298.75 K

0.33110.0576 0.0011 1.8105 0.3150 0.0016

0.62980.1096 0.0012 2.5344 0.4410 0.0022

0.91130.1586 0.0016 2.7797 0.4837 0.0017

1.27890.2225 0.0013 2.9941 0.5210 0.0017

1.54030.2680 0.0024

T = 313.58 K

0.16180.0221 0.0011 1.6413 0.2234 0.0024

0.54170.0737 0.0012 1.9669 0.2678 0.0017

0.98200.1337 0.0016 2.3695 0.3226 0.0015

1.25070.1702 0.0022 2.7381 0.3727 0.0021

Measurement and Prediction of the Solubility of CO in Ester Mixture

28 2

Table 5. Mole fraction (xi), equilibrium pressure (p), and

uncertainties (ui) of CO2 in DMC + propyl acetate from

282.86 K to 313.73 K.

p/MPa xi u

i p/MPa xi u

T = 282.86 K

0.1869 0.05167 0.0013 0.9840 0.2637 0.0012

0.3474 0.0979 0.0017 1.1182 0.2943 0.0019

0.5358 0.1481 0.0013 1.2986 0.3322 0.0021

0.7113 0.1922 0.0022 1.4800 0.3722 0.0015

0.8647 0.2324 0.0020 1.7335 0.4239 0.0017

T = 298.79 K

0.1627 0.0296 0.0009 1.5895 0.2894 0.0015

0.3892 0.0709 0.0017 1.7723 0.3227 0.0020

0.5476 0.0997 0.0016 2.0373 0.3713 0.0014

0.8071 0.147 0.0011 2.2797 0.4151 0.0019

1.0966 0.1997 0.0021 2.5771 0.4693 0.0013

1.3551 0.2467 0.0018

T = 313.73 K

0.2284 0.0324 0.0010 1.7740 0.2519 0.0011

0.5270 0.0748 0.0018 2.1766 0.3091 0.0022

0.7694 0.1093 0.0019 2.4870 0.3532 0.0021

1.0268 0.1458 0.0024 2.7946 0.3969 0.0015

1.3203 0.1875 0.0023

Figure 1. Vapor-liquid equilibrium of the CO2 + DMC +

propylene carbonate system in this study. x is the mole frac-

tion of CO2 in liquid-phase and p is the partial pressure of

CO2 at equilibrium state: ●, 282.81 K; ■, 298.69 K; ▲,

313.75 K.

It can be seen from Table 2 to Table 5 and Figure 1

to Figure 4, that the solubility of CO2 in the four mixed

solvents decreases with increasing temperature and de-

creasing pressure. And the solvent absorption capacity

Figure 2. Vapor-liquid equilibrium of the CO2 + DMC +

ethylene carbonate system in this study. x is the mole fraction

of CO2 in liquid-phase and p is the partial pressure of CO2

at equilibrium state: ●, 282.83 K; ■, 298.78 K; ▲, 313.75 K.

Figure 3. Vapor-liquid equilibrium of the CO2 + DMC +

diethyl carbonate system in this study. x is the mole fraction

of CO2 in liquid-phase and p is the partial pressure of CO2

at equilibrium state: ●, 282.89 K; ■, 298.75 K; ▲, 313.58 K.

Figure 4. Vapor-liquid equilibrium of the CO2 + DMC +

propyl acetate system in this study. x is the mole fraction of

CO2 in liquid-phase and p is the partial pressure of CO2 at

equilibrium state: ●, 282.71 K; ■, 298.79 K; ▲, 313.73 K.

depends on the gas partial pressure, which means that the

behavior of the mixed solvents used in physical absorption

also follows the Henry’s law. Henry’s law constants of

mixed solvents are listed in Table 6.

Searching a solvent with high CO2 absorption capacity

by experiment alone would probably be very expensive

and time consuming. [15] So this paper pays attention to

discuss some aspects which may affect the identification

Measurement and Prediction of the Solubility of CO2 in Ester Mixture

Table 6. Comparison of the Hildebrand parameter and

Henry’s law constant in DMC + diethyl carbonate system,

DMC + propyl acetate system, DMC + propylene carbonate

system and DMC + ethylene carbonate system at 298 K in

this study.

compound Hildebrand parameter of

the mixed solvent/Mpa1/2

Henry’s law

constant at 298

DMC + ethylene

carbonate 25.15 9.6612

DMC + propylene

carbonate 23.7 7.8270

DMC + diethyl

carbonate 19.1 5.7470

DMC + propyl

acetate 19 5.4909

and selection of a potential physical solvent for CO2

capture. The solubilization of a gas solute in a physical

solvent can be divided into two steps [16]: first, the in-

teractions among the solvent molecules must be broken

to provide some cavities which can accommodate the

solute molecules; second, the cavities formed in the first

step are then filled with solute molecules and new inter-

actions between the solute and solvent molecules are also

created. In previous studies, it had been discussed that

the ability to dissolve a gas solute of a solvent depended

mainly on the interactions among the solvent molecules.

[14] Thus, in this paper, the solvent – solvent interaction

is considered to be a main factor in solvent screening,

which can be described by Hildebrand solubility pa-

rameter of the solvent.

As can be seen from Table 6, the Henry’s law constant

clearly increases when the Hildebrand parameter increases,

which also illustrates CO2 solubility in physical solvents

increases with the decreasing of Hildebrand parameter.

This is mainly because in the gas dissolution process, the

greater of the Hildebrand parameter value, the stronger of

the solvent – solvent interactions, and the less cavities

which can accommodate the solute molecules. So in order

to increase the solubility of CO2, the interactions among

solvent molecules must be minimized as much as possible

which can create more cavities.

Furthermore, according to Hildebrand and Hansen

theory, [17-19] if the interactions between solute and

solvent can be neglected, Hildebrand solubility parameter

δ can reasonably used to describe and estimate the gas

solubility in solvent. A relationship between the loga-

rithm of the gas solubility and the Hildebrand solubility

parameter δ has been given by Hildebrand and other co-

workers, which can be described as follows: [20]

where δs is the solvent solubility parameter, δi is the dis-

solved CO2 gas solubility parameter, fi/fi,l is the ratio of

the fugacities of the CO2 gas in its pure gaseous state to

its hypothetical liquid state, Vi,l is the molar volume of

the hypothetical liquid. εs is the dielectric constant of the

solvent, α is the polarizability of the solute, and Q is the

quadrupole moment of the solute. For CO2 at 25, ℃Q =

4.1 × 10-26 e.s.u, α = 2.65 × 10-24 e.s.u, δi = 12.3 MPa1/2, Vi,l

= 55 × 10-6 m3 mol-1 and fi,l = 4.12 Mpa at 1 atm. [21] For

the mixed solvent, the parameter δs is replaced by δmixed.

 

,1exp

il il

fatpfatmRT



 (2)

mixeds,j s,j





 (3)

mixeds,j s,j





 (4)

where



s,j is the volume fraction of the solvent j, δs,j is the

solubility parameter of the pure solvent j and εs,j is the

dielectric constant of the pure solvent j.

But the Equation (1) cited in this paper is available

only at low pressure, bigger error of calculation occurs

when the pressure gets higher. It is obviously important

to consider the pressure impact on the application of

Equation (1). So some adjustment and modification

should be made to the equation, pressure correction items

were introduced in Equation (1), and a new equation was

proposed at high pressure in this paper, which can be

described as:

where A and B are two pressure correction factors.

Each value of the correction factors A and B for the four

mixed solvents are listed separately in Table 7.

The solvent added into the DMC can be divided into

two groups in this paper. Propylene carbonate and ethyl-

ene carbonate can be considered as a group of cyclic

compound, and propyl acetate and diethyl carbonate can

be classified as a linear compound group. As can be seen

in Table 7, the value correction factor B is about the

same, but the value correction factor A differs greatly for



,21 24

lnln10.12258.43 102.52 10

iiil ssi

xff Q









(1)



,21 24

lnln10.12258.43 102.52 10

iss i

fRT

 









BP

(5)

Measurement and Prediction of the Solubility of CO in Ester Mixture

30 2

different solvents. It is also found that the Henry’s law

constant decreases as the correction factor A increases.

Thus, the correction factor A brings about great influence

on the solubility prediction of carbon dioxide in liquid

solvent at high pressure. Table 7 also shows that in the

same group compound, the values of the correction factor

A are similar. But for the different group, the correction

factor A of the linear compound is larger than the cyclic

compound, which confirms the greater solubility of CO2

in linear compound mixed solvents. At the same time, it

can be seen from Figure 5, that under the same tempera-

ture, linear compound added can greatly improved the

solubility of CO2 in DMC, which also indicates the larger

of the correction factor A has a better absorption. In or-

der to verify the accuracy of the Equation (5), compari-

sons of the measured (xi) and calculated (xc) of the CO2

solubility in the four mixed solvents at 298 K were made

in Table 8 and Table 9.

5. Conclusions

Main conclusions of the study can be summarized as

follows:

Table 7. Correction factors of the DMC + diethyl carbonate

system, DMC + propyl acetate system, DMC + propylene

carbonate system and DMC + ethylene carbonate system at

298 K.

Mixed solvent A B

propyl acetate + DMC 0.7468 0.0673

diethyl carbonate + DMC 0.7126 0.0686

propylene carbonate + DMC 0.5230 0.0688

ethylene carbonate + DMC 0.4259 0.0687

Figure 5. Comparison of CO2 solubility in mixed solvent

system in this study. x is the mole fraction of CO2 in liq-

uid-phase and p is the partial pressure of CO2 at equilib-

rium state: ■, DMC + diethyl carbonate system, 298.75 K;

▲, DMC + propyl acetate system, 298.79 K; ●, DMC +

propylene carbonate system, 298.69 K; ●, DMC + ethylene

carbonate system, 298.78 K.

Table 8. Measured (xi) and calculated (xc) of the CO2 solu-

bility in DMC + diethyl carbonate system, DMC + propyl

acetate system at 298 K.

DMC + propyl acetate DMC + diethyl carbonate

xi x

c x

i x

0.0296 0.0296 0.0576 0.0575

0.0709 0.0708 0.1096 0.1095

0.0997 0.0997 0.1586 0.1586

0.147 0.1470 0.2225 0.2228

0.1997 0.1999 0.2680 0.2685

0.2467 0.2471 0.3150 0.3156

0.2894 0.2898 0.4410 0.4412

0.3227 0.3230 0.4837 0.4834

0.3713 0.3712 0.5210 0.5201

0.4151 0.4150

0.4693 0.4686

Table 9. Measured (xi) and calculated (xc) of the CO2 solu-

bility in DMC + propylene carbonate system and DMC +

ethylene carbonate system at 298 K.

DMC + propylene carbonate DMC + ethylene carbonate

xi x

c x

i x

0.0423 0.0422 0.0179 0.0179

0.0744 0.0744 0.0444 0.0443

0.1219 0.1220 0.0836 0.0836

0.1677 0.1680 0.1107 0.1108

0.2127 0.2132 0.1417 0.1419

0.2415 0.2419 0.1778 0.1781

0.2849 0.2852 0.2067 0.2071

0.3166 0.3168 0.243 0.2432

0.3537 0.3536 0.2685 0.2685

0.3971 0.3961 0.2818 0.2817

0.3204 0.3197

1) Under the pressure of 5 MPa and the temperature

variations from 282 K to 313 K, the solubility data

measured by constant-volume method of CO2 in

DMC + diethyl carbonate system, DMC + propyl

acetate system, DMC + propylene carbonate sys-

tem, and DMC + ethylene carbonate system de-

creases as temperature increases and pressure de-

creases.

Measurement and Prediction of the Solubility of CO in Ester Mixture31

2) The results show that CO2 solubility in physical

solvents increases with the decreasing of Hildebrand

parameter. The greater of the Hildebrand parameter

value, the stronger of the solvent – solvent interac-

tions, and the less cavities which can accommodate

the solute molecules.

3) It is also found by contrast that linear compound

has a greater ability to dissolve CO2 than the cyclic

compound at the same temperature. Furthermore,

the correction factor A brings about great influence

on the solubility prediction of carbon dioxide in

liquid solvent. This indicates that the correction

factor A can be regarded as an main impact factor

in the selection of a potential physical solvent for

CO2 capture.

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