International Journal of Greenhouse Gas Control 47 (2016) 8–16

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International Journal of Greenhouse Gas Control

journal homepage: www.elsevier.com/locate/ijggc

Carbon dioxide absorption in a packed column using imidazolium

based ionic liquids and MEA solution
Z. Ziobrowski, R. Krupiczka, A. Rotkegel ∗
Instytut Inżynierii Chemicznej Polskiej Akademii Nauk, Gliwice, Poland

a r t i c l e i n f o a b s t r a c t

Article history: The study of CO2 absorption in ionic liquids: [Emim][Ac], [Bmim][Ac] and 15 wt.% MEA solution in a packed
Received 29 May 2015 bed column is presented. Absorption column of inner diameter 0.05 m and 0.35 m length was filled with
Received in revised form Raschig rings ␾5 mm × 5 mm × 1 mm. Investigations were performed at atmospheric pressure what is
17 December 2015
important in the case of post combustion flue gases. The influence of mass transfer resistances in gas and
Accepted 13 January 2016
liquid phase as well as initial CO2 concentration and absorption temperature on CO2 removal efficiency
was investigated. In calculations the resistance in series model of the absorption process was applied.
Keywords:
The estimated values of enhancement factor of the reaction between CO2 and investigated liquids were
Carbon dioxide absorption
Ionic liquids (ILs)
used to predict mass fluxes of absorbed carbon dioxide for both ILs and MEA solution. The comparison of
Packed bed column experimental and calculation results show that in the same experimental conditions the investigated ILs
and MEA solution have comparable CO2 absorption capacities. The liquid side mass transfer coefficients
in the case of ILs are several times lower than for MEA solution. The research for new ILs characterized by
chemisorption mechanism, low viscosity and price is needed to take advantages of applying ionic liquids
in the process of CO2 separation in a packed column.
© 2016 Elsevier Ltd. All rights reserved.

1. Introduction
The growth in worldwide carbon dioxide emission from uti-
lization of fossil fuels is predicted to 40.2 GT by the year 2030
(International Energy Agency, 2011). Therefore, research endeavors
in developing new technologies for efficient and economic capture
and sequestration of large quantities of CO2 (Blatha et al., 2012;
Zhao et al., 2012).
A number of CO2 capture technologies used on laboratory and
industrial scale are processes based on physisorption or chemisorp-
tion, membrane separation, molecular sieves, carbamation, amine
physical adsorption, amine dry scrubbing, mineral carbonation,
absorption in ionic liquids (D’Alessandro et al., 2010).
Currently amine based – MEA (monoethanolamine), DEA
(diethanolamine), MDEA (methyldiethanolamine) scrubbing pro-
cesses are one of the most widespread techniques in industry
for post combustion CO2 capture (Rochelle, 2009; Budzianowski,
2015). The obstacles being reported are: insufficient CO2 capture
capacity, high solvent losses caused by evaporation, degradation
and poor thermal stability, as well as the equipment corrosion
(Hasib-ur-Rahmana et al., 2010; Zhao et al., 2011, 2012). The
∗ Corresponding author.
E-mail address: arot@iich.gliwice.pl (A. Rotkegel).
regeneration step may increase the total operating costs of the
capture plant up to 70%, especially for primary and tertiary amines
where the heat of reaction is quite high (Metz et al., 2005; Schäfer
et al., 2002).
As an alternative, ionic liquids (ILs) have been considered in the
recent years as solvents for CO2 absorption (Blatha et al., 2012;
Baltus et al., 2005). The properties of ionic liquids such as: thermal
stability, negligible vapor pressure, tunable physicochemical char-
acter, high CO2 solubility, more environmentally friendly character
make them attractive reversible CO2 capture absorbents. The low
IL heat capacity (one-third of that of aqueous systems) along with
diminished corrosion of the equipment may have profound effect in
reducing the high investment and operation cost (Yujiao Xie et al.,
2014; Mark et al., 2010; Perissi et al., 2006). An important drawback
in the case of ILs is their high viscosity and price.
In 2002 Bates et al. proposed the use of an amine function-
alized task specific ionic liquid (TSIL) for CO2 separation (Bates
et al., 2002). The loading capacity was similar to a MEA solution.
These investigations were supported by Bara et al. (2009a). Baltus
et al. (2004) determined solubility of CO2 in a series of imidazolium
based ILs at low pressure. It was found to increase with the length
of the alkyl side chain on the imidazolium ring. Wang et al. (2010)
found the formation of carboxylate at the imidazolium ring. The
carboxylate formation was also found by Maginn (2005), they just
used an ionic liquid containing an acetate anion.

http://dx.doi.org/10.1016/j.ijggc.2016.01.018
1750-5836/© 2016 Elsevier Ltd. All rights reserved.
 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16 9

the IL-MEA and MEA processes and found that the IL-MEA process
Nomenclature saves 15% regeneration heat duty compared to the MEA process.
Up today, the main research in CO2 solubility in [Cn mim][Ac]
A column fixed bed area (m2 ) was performed at laboratory scale (Mark et al., 2010; Huang et al.,
a specific packing area (m2 m−3 ) 2014; Yokozeki et al., 2008; Gurau et al., 2011; Khonkaen et al.,
C concentration of CO2 in gas phase 2014). [Emim][Ac] is promising ionic liquid for CO2 absorption.
D diffusivity (m2 s−1 ) Furthermore, its CO2 absorption ability can be improved by adding
d diameter (m) 20 wt.% of DBU (1,8-diazabicycloundec-7-ene) (Blatha et al., 2012).
E enhancement factor Simulation results of carbon dioxide capture from post combustion
F cross-section column area (m2 ) flue gases using [Emim][Ac] show lower energy requirements and
GL total mass of the liquid (kmol) higher investments cost of IL-based process compared to MEA-
H Henry’s law constant based process (Khonkaen et al., 2014). There are few pilot projects
h column length (m) for evaluating the ability of ionic liquids in progression, yet gas
k mass transfer coefficient (kmol m−2 s−1 ) capture data are not available. Ion Engineering Company possesses
Ka absorption constant demonstration facility and intended to use the knowhow of ionic
kCF reaction rate constant (kmol−1 s−1 ) liquids for industrial-scale sweetening of natural gas and flue gas
Kov overall mass transfer coefficient (kmol m−2 s−1 ) CO2 separation (Bara et al., 2009b; ION Engineering, 2009). AE&E
L bed length (m) (Austrian Energy & Environment) group also has plans to work on a
NCO2 absorption flux of CO2 (kmol m−2 s−1 ) pilot plant scale comparative study between MEA and task-specific
r reaction rate (kmol s−1 ) ionic liquids for post combustion CO2 capture (Austrian, n.d.).
Re Reynolds number Nevertheless, more study is needed to find out the best solution
s absorption capacity for CO2 capture systems (Hasib-ur-Rahmana et al., 2010; Ebner
Sc Schmidt number and Ritter, 2009).
Sh Sherwood number The mass transfer behavior for CO2 absorption into different
T temperature (◦ C) liquid solvents appears to be important for the process design.
V flow rate (kmol s−1 ) Weiland et al. (1982) examined the design of packed strippers and
x liquid molar fraction presented extensive set of mass transfer coefficient measurements
y gas molar fraction using packed column and MEA solution. Galan Sanchez et al.
(2011) analyzed kinetic results obtained for CO2 absorption in
Greek letters
amino-functionalized IL and MEA solutions. They found their
ε bed porosity
reactivity with CO2 comparable. Gómez-Coma et al. (2014) found
 mass transfer driving force viscosity (Pa s)
that overall mass transfer for CO2 absorption in ILs using hollow
 molar density (kmol m−3 )
fiber membrane contactor is controlled by the liquid side mass
 time (s)
transfer resistance.
ϑz equivalent linear dimension (m)
In this paper the study of CO2 capture in imidazolium based ILs
in a packed column is presented for low pressure which is impor-
Subscripts
tant in the case of post combustion flue gases. The packed columns
CO2 carbon dioxide
are the standard technical solution used in many industrial pro-
col column
cesses and currently predominant as the contactor of choice for
G gas
solvent stripping. However, limiting factors for the application of
i inert
this technology are its size and large capital cost.
in column inlet
The aim of the present work was to analyze and compare the
L liquid
relevance of mass transfer in the process of CO2 removal in a packed
m mean value along the diffusion path
column for ILs and 15 wt.% MEA solution. The results will allow to
out column outlet
determine the possible application of ILs in a packed column for
r Raschig ring
CO2 removal from post combustion flue gases.
[Emim][Ac] and [Bmim][Ac] were used owing to their chemical
Superscripts
absorption mechanism, predictable high CO2 absorption capacities,
* equilibrium state
known properties and production methods. Most of the up-to-
− average value of the inlet and outlet of the column
date tested ILs absorb CO2 physically. Using ionic liquids with a
dominant physical absorption mechanism leads to low loading
capacities compared to MEA solutions but also to easier desorp-
tion process (Blath et al., 2011; Strazisar et al., 2003; Feng et al.,
Shiflett et al. have performed simulation for a CO2 separa- 2012; Zhou et al., 2012). The chemical absorption of CO2 in ionic
tion process using [Bmim][Ac] as liquid absorbent and compared liquids containing a carboxylic anion can be an alternative to com-
with the MEA technology. They found that a process based on mon amine scrubbing processes to overcome their disadvantages
[Bmim][Ac] can replace a MEA-based scrubbing system in a coal (Blatha et al., 2012; Yokozeki et al., 2008; Gurau et al., 2011;
burning power plant (180 MW). The energy losses can be reduced Janiczek et al., 2012). There is still uncertainty or lack of experi-
by 16% and the investment costs are about 11% lower compared mental data whether to choose amine or IL based more efficient
to the MEA process (Mark et al., 2010). Basha et al. (2013, 2014) technology of CO2 capture.
developed a conceptual process for CO2 capture from the fuel
2. Experimental
gas streams produced in a 400 MWe IGCC power plant, in which
[Bmim][Tf2 N] and two TEGO ILs (compound mixtures supplied by 2.1. Setup
Evonik-Degussa GmbH Co., Hopewell, VA, USA) were used as liquid
absorbents. Their results showed that the studied ILs can be used The main part of the experimental setup, shown schemati-
as a physical solvent for CO2 capture. Huang et al. (2014) compared cally in Fig. 1 is a packed glass column (1), 0.35 m length, inner
10 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16
Fig. 1. Experimental setup. 1 – packed column, 2 – heating jacket, 3 – packed bed,
4 – vessel, 5 – pump, 6 – thermostat.
diameter 0.05 m, equipped with water jacket (2). The column was
filled with Raschig rings of 5 mm × 1 mm diameter and 5 mm length
(a = 546 m2 /m3 , ε = 0.6527). The ionic liquid is introduced on the top
of the column, flows through packing and absorbs carbon dioxide
from gas (cocurrent or countercurrent flow). The mixture of CO2
and ionic liquid is gathered in a vessel (4) from which it is returned
to the top of column (1) by means of a pump (5). The column was
thermostated by Thermostat Lauda Eco Gold (6).
The temperatures of the liquid at the top of the column and
at the bottom of the vessel (4) were measured by NiCr-Ni ther-
mocouples. The gas flow rates were measured by flow meter and
rotameters. Liquid flow rate was regulated by peristaltic pump
Masterflex. Pure gases (99.99%) were supplied by Air Products.
The inlet and outlet CO2 concentrations were measured with
Madur GA-40 T plus (IR). The used imidazolium based ionic liquids
were 1-ethyl-3-methylimidazolium acetate ([Emim][Ac]) and 1-
Butyl-3-methylimidazolium acetate ([Bmim][Ac]) purchased from
Sigma–Aldrich. Pure MEA was supplied by POCh Gliwice and mixed
with distilled water to obtain 15 wt.% solution.
2.2. Methodology
The separate CO2 absorption experiments for pure [Bmim][Ac],
[Emim][Ac] and 15 wt.% MEA-water solution were performed in the
same experimental conditions (absorption temperature, gas and
liquid flow rate, initial CO2 concentration, cocurrent or countercur-
rent flow, atmospheric pressure to determine and compare the CO2
absorption efficiency in a packed column for investigated liquids.
The setup was preheated and operated in experimental condi-
tions until liquid flow and temperature were stabilized (about 1 h).
The gas mixture (N2 and CO2 ) was prepared by mixing pure carbon
dioxide and nitrogen in a column filled with ceramic packing. At
the start of measurements the prepared and preheated gas mixture
with constant CO2 concentration was introduced on top (or at the
bottom) of the column. The CO2 inlet and outlet gas concentrations,
pressure drop, liquid and gas temperatures and flow rates were
measured until liquid was saturated (Cout /Cin = 0.90–0.98, 2–4 h).
After each experiment the IL was regenerated by desorption in the
temperature of 90 ◦ C. The pure nitrogen was used as an inert gas to
help stripping CO2 (6–8 h). The desorption process was controlled
gravimetrically. The mass decrease was measured every hour and
desorption process was carried out until the mass changes were
negligible (0.1 g). In case of MEA solution for each experiment new
mixture was prepared. At each liquid change the setup was rinsed
with water and ethanol then air dried.
2.3. Testing plan and parameters
To evaluate the application of ILs for CO2 absorption in a packed
column the CO2 removal efficiency and absorbed CO2 mass fluxes
for both ILs and MEA solution should be determined and com-
pared. In experiments the effect of different gas and liquid flow
rates, absorption temperatures, inlet CO2 concentration in gas mix-
ture as parameters as well as the effect of liquid–gas flow direction
(cocurrent or countercurrent) were investigated.
2.4. Testing operating conditions
Prices of 1 kg of ILs are 868 D and 883 D for [Emim][Ac] and
[Bmim][Ac] respectively. For comparison the cost of 1 kg pure MEA
is 28 D . Because the investigated ILs are expensive, a small glass col-
umn (0.35 m length, inner diameter 0.05 m) was chosen and initial
hydraulic test were carried out with 98.5 wt.% glycerol–water mix-
ture of comparable viscosity with ([Emim][Ac]). Different packings
were tested: ceramic Berl saddles (4 mm length, 3 mm height), steel
springs (3 mm length, 3.5 mm diameter) and glass Raschig rings
(10 mm × 1 mm diameter and 10 mm length and 5 mm × 1 mm
diameter and 5 mm length). It was found that the best flow con-
ditions were obtained for Raschig rings of 5 mm × 1 mm diameter
and 5 mm length. For this packing the gas and liquid flow rates
were determined for which the column worked correctly: all pack-
ing was wet, liquid was evenly distributed without dry spots or
flooding. Good flow conditions were found for liquid flow in the
range 0.05–0.5 l/min and for gas flow in the range 1.3–2.3 l/min.
Based on testing results, it was found that CO2 absorption in
[Emim][Ac] and [Bmim][Ac] may be carried out in a limited range
of flow rates: 0.05–0.5 l/min for liquid and 1.3–2.3 l/min for gas
in cocurrent flow and 0.05–0.1 l/min for liquid and 1.3–2 l/min for
gas in countercurrent flow. For higher flow rates the column was
flooded.
The absorption temperature should be as low as possible,
because it determines the absorption capacity of investigated liq-
uids and efficiency of CO2 capture. Initial tests showed that CO2
absorption process carried out in temperature 30 ◦ C leads to solid-
ification of [Bmim][Ac]. The CO2 absorption process in a packed
column using imidazolium based ionic liquids and MEA solution
was carried out in the temperature of 40 ◦ C. Some experiments
were performed in the temperature of 60 ◦ C to find out the effect of
absorption temperature on the investigated process. The inlet CO2
concentrations in gas mixture were chosen respectively: 4.5, 9, 5,
14.5, 20.9 vol.%. Generally the CO2 concentration in post combus-
tion flue gases is in the range 12–15 vol.%.
2.5. Sampling method and accuracy of measurements
The measurements were done in experimental series. Exper-
imental series were obtained by measuring inlet and outlet CO2
concentrations (Cin , Cout ) in specified time periods for both ILs
and MEA solution in the same experimental conditions (liquid and
gas flow rate, inlet CO2 concentration, absorption temperature,
liquid–gas flow direction, atmospheric pressure). The experiments
were carried out up to outlet CO2 concentration in gas phase
Cout /Cin = 0.90–0.98.
 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16 11

The measured values were presented as concentration or effi-

ciency data (Figs. 2 and 3) or CO2 removal efficiency profiles
(Figs. 5–12).
Liquid flow rates were measured with accuracy ±2 ml/min and
gas flow rates ±20 ml/min. Temperature of the thermostated col-
umn was measured with resolution 0.01 ◦ C and absolute accuracy
±0.2 ◦ C. The temperatures were measured by NiCr-Ni thermocou-
ples with accuracy ±0.2 ◦ C. The inlet and outlet CO2 concentrations
were measured with accuracy ±0.01 vol.%.

2.6. Limitation of experimental setup

Used ILs are expensive and their viscosities are very high (0.081
and 0.203 Pa s for [Emim][Ac] and [Bmim][Ac] respectively in 40 ◦ C
(Fendt et al., 2011)). Because of prices and viscosities of investigated Fig. 3. The effect of liquid flow rate and initial CO2 concentration in gas mixture on
CO2 removal efficiency.
ILs experimental setup limitations need to be taken into account.
Laboratory scale apparatus was made up to accommodate about
1 kg of IL. The small column (0.35 m length, 0.05 m diameter)
together with chosen packing (convenient ratios dcol /dr = 10 and
L/dcol = 7) allows to obtain correct liquid–gas flows. However single
passing of the liquid through the column gives only small changes
in CO2 concentrations in liquid. For practical reasons the residence
time should be longer to enable greater saturation of the liquid
passing through the column and improve the efficiency of the pro-
cess. The bigger column should allow to obtain higher CO2 removal
efficiency due to longer residence times and lower flow resistances.
High viscosity of investigated ILs allows only for limited ranges of
flow rates in case of small column. For laminar flow the length of the
column (0.35 m) was enough to establish flow profiles and obtain
evenly distributed liquid film.

3. Experimental results

The experimental results are shown in Figs. 2–8. The efficiency

of CO2 removal is defined as:
Cout
ef = 1 −
Cin
The ratio Cout /Cin represents outlet dimensionless concentration
of CO2 in gas phase after passing through the packed column. At the
beginning of each experiment the values of carbon dioxide concen-
tration Cout in a gas phase are low due to the absence of CO2 in a
liquid phase. After respectively long time the ratio Cout /Cin ∼
= 1, the
liquid is saturated and absorption process stops.
3.1. Effect of gas and liquid flow rates
Fig. 4. The effect of CO2 concentration in inlet gas on CO2 removal efficiency profile
for T = 40 ◦ C.
(1)
efficiency of carbon dioxide removal (ef ) are shown for [Emim][Ac].
Outlet CO2 concentrations presented in Figs. 2 and 3 were measured
at the experiment initial stage ( = 3 min) in absorption tempera-
ture 40 ◦ C, gas flow rate 2.3 l/min and for cocurrent flow of gas and
liquid.
The measured values are compared in four experimental series
for different inlet CO2 concentrations: 4.5, 9.5, 14.5, 20.9 vol.%
and different liquid flow rates: 0.05, 0.1, 0.2, 0.4, 0.5 l/min. For

In Figs. 2 and 3 the effect of liquid flow rate and initial CO2
concentration in gas phase on outlet CO2 concentration (Cout ) and

Fig. 2. The effect of liquid flow rate and initial CO2 concentration in gas mixture on Fig. 5. The effect of absorption temperature on CO2 removal efficiency for
outlet CO2 concentration. Cin = 15 vol.%.
12 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16
Fig. 6. The effect of co- and countercurrent flow on CO2 removal efficiency profile
[Emum][Ac] in temperature 40 ◦ C.
Fig. 7. The effect of co- and countercurrent flow on CO2 removal efficiency for MEA
15 wt.% in temperature 40 ◦ C.
each experimental series CO2 outlet concentration decreases with
increasing liquid flow rate (Fig. 2), which is caused by better mix-
ing and higher Re numbers. Rising liquid flow rates lead to greater
amounts of CO2 absorbed in IL and consequently more efficient CO2
removal (Fig. 3).
Fig. 8. Comparison of CO2 removal efficiency profiles for [Emim][Ac], [Bmim][Ac]
and 15 wt.% MEA.
With rising inlet CO2 concentration in gas mixture in the range
4.5–20.9 vol.% the inlet CO2 mass flux in gas mixture is rising while
absorbed CO2 mass flux in liquid is the same (unchanged experi-
mental conditions). As a result measured outlet CO2 concentrations
in gas mixture were greater (Fig. 2) and efficiency of CO2 removal
was lower (Fig. 3).
The same relationship was observed in experiments performed
for countercurrent liquid–gas flow. In this case available liquid flow
rates were limited to 0.05–0.1 l/min.
The measured effect of gas flow rate on outlet CO2 concentration
(Cout ) and efficiency of carbon dioxide removal (ef ) was negligible
for investigated liquids.
3.2. Effect of inlet CO2 concentration in gas phase and absorption
temperature
In Figs. 4 and 5 the effect of inlet CO2 concentration in gas
phase and absorption temperature on CO2 removal efficiency is
shown for [Emim][Ac] and cocurrent flow. For low inlet CO2 con-
centration (5 vol.%) only small changes in the efficiency profile were
observed, while for higher inlet CO2 concentration (15 vol.%) the
efficiency changes are more significant and it takes more time to
reach the outlet CO2 concentration in gas Cout /Cin = 0.95 (ef = 0.05)
at the absorption temperature 40 ◦ C (Fig. 4). In Fig. 5 the efficiency
for higher absorption temperature 60 ◦ C and 15% inlet CO2 concen-
tration is lower and decreases faster than for 40 ◦ C and 15% inlet
CO2 concentration.
Carbon dioxide solubility depends on the absorption temper-
ature. For lower absorption temperature the amount of absorbed
CO2 in IL is bigger and thus the efficiency is higher.
3.3. Effect of cocurrent and countercurrent flow
The experiments performed in countercurrent flow show that
the measured CO2 removal efficiencies are lower than in case of
cocurrent flow for both investigated ILs and MEA solution. Addi-
tionally, in countercurrent flow the flooding of the column begins
at lower gas and liquid flow rates.
Experiments carried out in the same conditions both for ILs and
MEA solution show better mass transfer in cocurrent flow. It may
be caused by different hydrodynamic conditions, different passing
times of CO2 bubbles through the bed and different flow patterns.
3.4. Comparison of CO2 removal efficiencies
In Fig. 8 experimental results of carbon dioxide absorption for
[Bmim][Ac], [Emim][Ac] and 15 wt.% MEA solution are compared in
the same conditions: cocurrent flow, inlet CO2 concentration equal
15 vol.% and temperature T = 40 ◦ C.
For both ionic liquids the initial CO2 removal efficiency is sig-
nificantly lower than for 15 wt.% MEA solution. For MEA solution
the initial efficiency starts from ef = 0.96 compared to ef = 0.28 for
[Emim][Ac]. Looking at the trajectory of experimental points the
CO2 removal efficiency for MEA solution decreases faster to reach
the outlet CO2 concentration ratio Cout /Cin = 0.95 (ef = 0.05) after
about 80 min instead of 210 min for [Emim][Ac] and 135 min for
[Bmim][Ac].
Gómez-Coma et al. (2014) obtained higher CO2 removal effi-
ciencies for [Emim][Ac] using hollow fiber membrane contactor.
They found that temperature influence is significant in case of
[Emim][Ac].
4. Mass transfer model
When CO2 is absorbed in aqueous MEA solutions or in ILs,
the chemical reaction takes place. For aqueous MEA solutions the
 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16 13

overall reaction mechanism with carbamate formation has been calculate the mass fluxes of absorbed CO2 in both ILs and MEA
extensively studied and is well understood (Hikita et al., 1977; solution.
Versteeg et al., 1996). Model assumptions and simplifications:
For ILs containing anion [Ac]− , such as [Emim][Ac] and
[Bmim][Ac] it was found that absorption of carbon dioxide is much • Reaction with CO2 is regarded as pseudo first order with respect
more promising due to its dominant chemical absorption character to CO2 .
(Blatha et al., 2012). The suggested reaction mechanism with car- • Process take places under isothermal and isobaric conditions.
boxylate formation was proposed by Maginn (2005). The acetate • Gas–liquid equilibrium is preserved at the interface.
anion deprotonates the [Emim]+ , [Bmim]+ cation at C(2) atom of • According to film theory mass transfer resistance occurs only in
imidazolium ring. The dissolved carbon dioxide reacts with the neg- a thin layer adjacent to the interface.
atively charged atom to a stable carboxylate. For [Bmim][Ac] the • Enhancement factor E used to calculate the mass fluxes of
mechanism seems even more complicated, because the solubility absorbed CO2 in either ILs or MEA solution was estimated from
results from two distinct regimes (Shiflett et al., 2008; Cabaco et al., experimental data.
2012). The first regime is dominated by the chemical reaction with
carboxylate formation which corresponds to a CO2 mole fraction Mass transfer flux can be calculated from the mass balance of
less than 0.35. The second regime, in which carboxylation reaction the gas phase:
is stopped, is dominated by physical absorption.  
The concentration of ionic liquid can be considered unchanged VG ȳ − Ka x̄
NCO2 = (y − yout ) = Kov (7)
upon initial CO2 absorption, hence reaction with CO2 may be A in ȳi,m
regarded as pseudo first order with respect to CO2 (Galan Sanchez
et al., 2011). When the chemical reaction in liquid phase takes place For gas and liquid flowing through the packed column, the CO2
the mass transfer is enhanced. The enhancement factor E is the mass transfer fluxes at the interface are equal and can be calculated
ratio between the mass flux in the presence of reaction and mass from:
flux when only physical absorption takes place. A resistance-in-    
series model (Gómez-Coma et al., 2014; Shulman et al., 1955; Luis x̄ − x̄∗ ȳ∗ − ȳ
NCO2 = kG = EkL (8)
et al., 2009) was used to obtain the relation between the overall x̄i,m ȳi,m
mass transfer coefficient, Kov , and a combination of gas side, kG ,
In order to obtain the CO2 concentration profiles in gas and liquid
and liquid side, kL mass transfer coefficients.
a differential Eq. (9) should be solved. On each step of integration
Taking into account the chemical reaction in the liquid
the concentration yout was calculated in accordance with Eq. (7)
(expressed by the enhancement factor, E) the equation is as follows:
and CO2 mass flux NCO2 was calculated iteratively from Eqs. (7) and
1 1 H (8).
= + (2)
Kov kG EkL
dx ANCO2
where kG and kL are the individual mass transfer coefficients in the =
d GL
gas and liquid film, respectively. E is the enhancement factor of the (9)
with boundary condition
chemical reaction of CO2 in the liquid phase. H is the Henry’s law
constant, which in this work was defined as: =0→x=0

y∗ G Consequently carbon dioxide concentration in time can be cal-

H= (3)
x∗ L culated as:
 
where the ratio of CO2 molar fraction in gas and liquid represents ANCO2
the absorption constant Ka x() = d (10)
0
GL
y∗
Ka = (4) The vapour–liquid equilibrium data of CO2 in [Emim][Ac],
x∗
[Bmim][Ac] are reported in the literature by Shiflett et al. (2008),
The enhancement factor (E) from simplified DeCoursey (1982) Shiflett and Yokozeki (2009) and for MEA solution by Aronu et al.
solution in the case of pseudo first order reaction in IL’s and aqueous (2011).
MEA solution is defined by expression: Mass transfer in liquid phase kL was calculated based on equa-
 tion for laminar and transition range (Sherwood et al., 1952):
E= 1 + Ha2 (5)
 ϑ 1/2
z
where Hatta number Ha can be expressed as a ratio of diffusion and ShL = 3.76Re−1/3 for Re2/3 Sc 1/2 < 5.17
h
reaction times.
  ϑ 1/2  ϑ 1/2
Ha2 = diffusion (6) ShL = 0.725Re1/3 Sc 1/2
z
for Re2/3 Sc 1/2
z
> 5.17
reaction h h
(11)
Large value of Hatta number implies that diffusion time is much
longer than reaction time and hence considerable reaction takes
place in the film. Based on the penetration theory, when both mass The diffusivities of carbon dioxide absorbed in imidazolium
transfer and reaction take place, Hatta number (Ha) is used to relate based ionic liquids are calculated according to Morgan et al. (2005):
the mass transfer and the reaction rate (Vesterterp et al., 1987).
1
The main objective of the mathematical model was to describe DCO2 = 2.66 × 10−3 1.04
(12)
the process of CO2 absorption accompanied by the chemical reac- 0.66
2
V̄¯ 1
tion in a packed column, using enhancement factor E as a parameter
of the model. Because of the lack or unreliability of literature data where 2 is the viscosity of ionic liquid in cP and V1 is the molar
concerning kinetic constants of CO2 reaction with IL the values of volume of CO2 at the normal boiling point (33.3 cm3 /mol). The dif-
enhancement factor E estimated from experiments were used to fusivity is obtained in cm2 /s.
14 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16
Table 1
The physical parameters of the CO2 absorption process in a packed column.
Liquid  (kg/m3 ) × 103 (Pa s) DCO2 × 1010 (m2 s−1 )
[Emim][Ac] 1.025 66.98 4.21
[Bmim][Ac] 1.050 145.3 2.51
15% MEA 0.999 0.938 22.4
The diffusivities of carbon dioxide absorbed in MEA solution are
calculated according to Wilke Chang equation (Bird et al., 2002):
0.5
(
2 M2 ) T kG were calculated according to Eqs. (10)–(13), experimental ini-
DCO2 = 7.4 × 10−8
2 V10.6
where 2 ,M2 are the viscosity in cP and molecular weight in g/mol
of the solvent, ϕ is the association factor for the solvent, V1 is the
molar volume of CO2 at the normal boiling point (33.3 cm3 /mol)
and T is the temperature in K. The diffusivity is obtained in cm2 /s.
Mass transfer in gas phase kG was calculated from Van Krevelen
and Hoftijzer (Bird et al., 2002) equation:
Sh = 0.11Re0.8 Sc 0.33
5. Calculation results and discussion
Based on model Eqs. (2)–(14) the MATLAB calculation program
was designed. Input data for calculations were: gas and liquid flow
rate, input CO2 concentration in gas phase, and initial CO2 concen-
tration in liquid phase (usually equal 0), temperature of gas and
liquid phase and duration of the process. The calculations results
were presented as CO2 concentration profiles in liquid and outlet
gas.
The calculation results were presented as CO2 concentration
profiles in liquid and outlet gas. The outlet CO2 concentration pro-
files were calculated by integration of Eq. (9) with estimated values
of enhancement factor as a parameter of the model. The integra-
tion was achieved using ode45 – the standard MATLAB solver for
system of nonstiff differential equations. Ode45 algorithm is based
on the explicit Runge-Kutta (4,5) formula. Calculations were per-
formed with relative and absolute tolerance set to 1E-6. On each
step of integration outlet gas concentration (yout ) and CO2 mass
flux (NCO2 ) were calculated, taking into account equality of mass
fluxes in both phases according to Eq. (8). Eq. (8) was solved using
MATLAB function fsolve with both termination tolerance on the
function value (TolFun) and termination tolerance on X (TolX) set
to 1E-9. The mass flux profiles were determined according to Eqs.
(7) and (8).
Absorption constant Ka was calculated according to Eq. (4) from
literature data of CO2 solubility in ILs and MEA solution. For MEA
solution Ka constant was calculated from equilibrium solubility
of CO2 in aqueous 15 wt.% MEA in 40 ◦ C by Aronu et al. (2011).
They presented gas–liquid equilibrium data as a relation between
pressure in gas phase and loading ratio ˛. Using these data molar
fraction in gas phase (y* ) was calculated as ratio of CO2 partial and
total pressure, and molar fraction in liquid phase (x* ) was calculated
from CO2 loading ratio (˛).
For ILs analogous calculations were performed for CO2 molar
fraction in gas and liquid phase (y* ,x* ) based on literature data of
CO2 equilibrium solubility in ILs by Shiflett et al. (2008).
In calculations absorption constant Ka was in the range 0.02–0.8
for [Bmim][Ac], 0.03–2.5 for [Emim][Ac] and 0.2–4.4 for 15 wt.%
MEA solution.
In Table 1 the physical parameters of the CO2 absorption process
in packed column are compared. All parameters are calculated for
the same experimental conditions: temperature 40 ◦ C, cocurrent
flow, inlet CO2 concentration 15 vol.%.
kL × 108 (kmol m−2 s−1 ) kG × 105 Nexp, = 0 × 106 s (kg/kg)
(kmol m−2 s−1 ) (kmol m−2 s−1 )
9.90 3.08 0.166 0.053
6.04 3.08 0.177 0.043
204 3.08 0.668 0.049
Densities listed in Table 1 are taken from manufacturer speci-
fication, IL’s and MEA solution viscosities were found in literature
(Fendt et al., 2011; Meng-Hui and Yei-Chung, 1994). DCO2 , kL and
(13)
tial mass flux of CO2 Nexp, = 0 were calculated from Eq. (6) and
maximal sorption capacity s was taken from our experiments on
CO2 absorption in ILs and MEA solution in bubble apparatus. As it
can be seen viscosities of both ILs are significantly higher than for
MEA solution. As a consequence the diffusivity and mass transfer
coefficients in liquid phase for both ILs are much lower. The calcu-
lated mass transfer coefficients in liquid and gas phase show that
the CO2 absorption process in a packed column is controlled by
(14) liquid side mass transfer resistance. Gómez-Coma et al. (2014) and
Luis et al. (2009) confirmed higher resistance to mass transfer when
IL was used. They obtained overall mass transfer coefficients using
a hollow fiber membrane contactor.
The liquid side mass transfer coefficient and initial mass flux of
CO2 in the case of ILs are several times lower than for MEA solu-
tion. Absorption capacities s (mass of absorbed CO2 per mass of the
liquid) are comparable in the same experimental conditions for all
investigated liquids.
Calculated values of CO2 outlet concentrations in gas phase were
compared with experimental ones in Figs. 9–11. Additionally the
calculated CO2 concentration profiles in liquid phase are presented.
The calculated and experimental values of CO2 outlet concentra-
tions for [Emim][Ac], [Bmim][Ac] and MEA solution are presented
for the same experimental conditions: cocurrent flow, inlet CO2
concentration 15% and T = 40 ◦ C. For both ionic liquids and MEA
solution the calculated and experimental values of the outlet CO2
concentration are in good agreement.
The calculated and experimental values of mass fluxes were
compared in Fig. 12 taking into account enhancement factor of the
chemical reaction of CO2 in the liquid phase. Because of unreliability
of literature data concerning kinetic constant of reaction between
CO2 and investigated ILs, enhancement factor (E) was estimated
from our experimental data. The estimated values of enhancement
factor (E) allow to predict mass fluxes of absorbed carbon diox-
ide with good accuracy for both ILs and MEA solution in the same
Fig. 9. Comparison of experimental and calculation CO2 concentrations for
[Bmim][Ac].
 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16
Fig. 10. Comparison of experimental and calculation CO2 concentrations for
[Emim][Ac].
Fig. 11. Comparison of experimental and calculation CO2 concentrations for 15%
MEA solution.
experimental conditions. The calculated values of E are in good
agreement with the ones found in literature. For CO2 absorption
in MDEA solutions in bubble column reactor an enhancement fac-
tor was found to be about 15 by Navazza et al. (2009) for initial
MDEA concentration 1 mol/l and absorption temperature 25 ◦ C. The
enhancement factor for temperature 40 ◦ C, and MEA concentra-
tion 3 M (18.3 wt.%) was reported by Meldon and Morales-Cabrera
(2011). They found that for film thickness 5 ␮m (typically for a
packed tower) E ∼ = 20. For CO2 absorption in [Emim][Ac] in the
Fig. 12. Comparison of experimental and calculation CO2 absorption mass fluxes.
15
Fig. 13. Scattering of experimental and calculation results of CO2 removal efficiency.
polypropylene hollow fiber membrane module the enhancement
factor was found to be about 51 in temperature 45 ◦ C (Gómez-Coma
et al., 2014).
The calculated and measured CO2 initial mass fluxes for 15 wt.%
MEA solution (Fig. 4, Table 1) are about 4 times greater than
obtained for both investigated ILs. Mass flux of absorbed CO2 in
MEA solution decreases faster with time than for investigated IL’s.
The CO2 absorbed mass fluxes for [Bmim][Ac] and [Emim][Ac] are
comparable.
The scattering of calculated and experimental values of CO2
removal efficiency for both ILs and MEA solution is in the range
of ±20%, Fig. 13.
6. Conclusions
[Bmim][Ac] and [Emim][Ac] can be used for removal of carbon
dioxide from post combustion gases in investigated small packed
column only in the limited range of liquid and gas flow rates. The
operating flow rates (1.3–2.3 l/min for gas and 0.05–0.5 l/min for
liquid) were in laminar and transition regime. For higher flow rates
the column was flooded.
The efficiency of CO2 absorption depends on absorption temper-
ature and initial CO2 concentration in gas mixture (Figs. 2 and 3).
In the same experimental conditions [Bmim][Ac] and
[Emim][Ac] have comparable CO2 absorption capacities with
MEA solution (Table 1). However, ILs need much longer times
to remove the same amount of carbon dioxide from gas mixture
(Fig. 12).
The comparison of experimental and calculation results, based
upon the proposed model, shows that main mass transfer resis-
tance is in the liquid phase for both investigated ILs and MEA
solution. The liquid side mass transfer coefficients and initial mass
flux of CO2 in the case of ILs are several times lower than for MEA
solution (Table 1).
The estimated values of enhancement factor allow to predict
with good accuracy the absorbed CO2 mass fluxes in a packed col-
umn for either ILs or MEA solution (Fig. 12).
Studying the transport phenomena is important for the suitable
design and operation of industrial units used for CO2 capture with
ionic liquids, especially at low pressure like flue gas from coal-fired
power plants. Mass production of inexpensive ionic liquids char-
acterized by increased stability, low equipment corrosion and low
viscosities may allow for the application of ILs on a larger scale.
16 Z. Ziobrowski et al. / International Journal of Greenhouse Gas Control 47 (2016) 8–16
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