Int. J. Environment and Pollution, Vol. 51, Nos.

1/2, 2013 121

Modelling and simulation of reaction kinetics of

carbon dioxide absorption into aqueous ammonia in
a wetted wall column

Ujjal K. Ghosh* and Su Ching Yee

Department of Chemical Engineering,
School of Engineering and Science,
Curtin University,
CDT 250, 98009 Miri, Sarawak, Malaysia
Fax: +60 85 443837
E-mail: ujjalche@gmail.com
E-mail: ujjal@curtin.edu.my
E-mail: chingyee.amysu@gmail.com
*Corresponding author

Abstract: Carbon dioxide accounts for about 80% of all greenhouse gases
(GHG) and thus becomes the major source responsible for global warming
which is considered as the greatest environmental challenge the world is facing.
The post-combustion capture is the main way to lower the emission of existing
power plants and future power plants where CO2 is produced during the
combustion. Solvent-based CO2 capture technology a proven technology for
CO2 capture. Carbon dioxide absorption process using an ammonia solution
provides many advantages including higher absorption capacity, no degradation
and lower regeneration energy requirement. In this paper, a mathematical
model for the reaction kinetics of carbon dioxide absorption into aqueous
ammonia in a wetted wall column is developed. Simulation of the mathematical
model is performed and the simulated results are compared with literature data.

Keywords: absorption; carbon dioxide; aqueous ammonia; wetted wall

column; carbon capture.

Reference to this paper should be made as follows: Ghosh, U.K. and Yee, S.C.
(2013) ‘Modelling and simulation of reaction kinetics of carbon dioxide
absorption into aqueous ammonia in a wetted wall column’, Int. J. Environment
and Pollution, Vol. 51, Nos. 1/2, pp.121–138.

Biographical notes: Ujjal K. Ghosh is currently a Senior Lecturer at the

Department of Chemical Engineering, Curtin University, Malaysia campus. He
finished his PhD from Indian Institute of Technology, Kharagpur, India before
joining the Department of Chemical and Biomolecular Engineering, University
of Melbourne Australia as a Postdoctoral Research Fellow to work on carbon
sequestration project.

Su Ching Yee finished her Bachelor degree in Chemical Engineering from

Curtin University, Malaysia campus. She is currently working as a Production
Engineer in a margarine and frozen dough manufacturing company based in
Singapore.

Copyright © 2013 Inderscience Enterprises Ltd.

122 U.K. Ghosh and S.C. Yee

1 Introduction

The main sources of carbon dioxide emissions are mainly from the combustion of fossil
fuels. Among all fossil fuels, coal is the main energy source and coal-fired plant is
distributed widely across the Earth’s surface (Oexmann et al., 2008). All of these coal-
fired plants discharge a huge amount of carbon dioxide into the atmosphere and amount
of carbon dioxide rises dramatically every year. Due to their low cost, availability,
existing reliable technology for energy production, and energy density, fossil fuels
currently supply over 85% of the energy needs of the USA and a similar percentage of
the energy used worldwide (EIA, 2006a, 2006b).
Many development and research activities have been done in the field of carbon
capture and storage (CCS) due to rise of awareness of the greenhouse effect or climate
change. The implementation of CCS allows the use of fossil fuels and coals as a source of
energy while in the mean time reduce the emissions of greenhouse gases (GHG) into the
environment. In CCS, carbon dioxide is removed from plant and stored securely in
reservoir. CCS is an integrated process which made up of three parts; carbon capture,
transport and storage. Carbon dioxide in flue gases is removed by capture technology and
transport to storage location via pipelines. The first step of CCS is capturing carbon
dioxide from flue gases. Currently, the main strategies for the carbon dioxide capture in a
fossil fuel combustion process are post-combustion capture, pre-combustion capture and
oxy-fuel combustion (Davidson and Metz, 2005). For each combustion process, a
different method of capturing CO2 produced as a by-product of energy production.
1 Post-combustion capture: In post-combustion capture, CO2 is separated from the flue
gas emitted after the combustion of fossil fuels from a standard gas turbine combined
cycle, or a coal-fired steam power plant. CO2 is being separated at relatively low
temperature, from a gaseous stream at atmospheric pressure and with low CO2
concentration (ca. 5–25% if air is used during combustion). Minor amounts of SO2,
NO2 and O2 may also be present. This possibility is by far the most challenging since
a diluted, low pressure, hot and wet CO2/N2 mixture has to be treated. Nevertheless,
it also corresponds to the most widely applicable option in terms of industrial sectors
(power, kiln and steel production for instance). Moreover, it shows the essential
advantage of being compatible to a retrofit strategy (i.e., an already existing
installation can be, in principle, subject to this type of adaptation) (Favre, 2007).
2 Pre-combustion capture: In pre-combustion capture the conversion of the fuel is
performed to a mixture of H2 and CO (syngas mixture) through partial oxidation,
steam reforming or auto-thermal reforming of hydrocarbons, followed by water-gas
shift reaction. The separation of CO2 (at 30–35%) from the H2 that is then fed as
clean fuel to turbines. In these cases, the CO2 separation could happen at very high
pressures (up to 80 bar of pressure difference) and high temperatures (300–700oC).
3 Oxy-fuel combustion: First step of oxy-fuel combustion is separation of
oxygen/nitrogen on the oxidant stream, so that a CO2/H2O mixture is produced
through the combustion process. The advantage of feeding an oxygen-enriched gas
mixture (95% oxygen) instead of air, is the achievement of a purge stream rich in
CO2 and water with very low N2 content, therefore the CO2 can be easily recovered
after the condensation of the water vapour.
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 123

However, CCS is still facing some challenges towards a full-scale demonstration and
commercialisation. Besides the technical and economic issues, CCS also faces to safety
and regulatory issues when dealing with the way of transport and storage of carbon
dioxide after the capturing process (Oexmann et al., 2008). These challenges need to be
overcame before CCS can be fully commercialised and minimise the concentration of
carbon dioxide within the atmosphere.
As mention before, in post-combustion capture process, carbon dioxide is separated
from the flue gas by chemical solvents absorption. In the absorption process, carbon
dioxide contained gas stream is dissolved in the chemical solvent, while at the mean time,
other gases remain in the gas stream and are not absorbed by the solvent. Typical
industrial process of carbon dioxide absorption and regeneration system can be
represented in Figure 1. The absorption and regeneration system consists of an absorber
and regenerator. In the absorber, carbon dioxide is removed from the gas stream by
contacting counter-currently with chemical solvents. The chemical solvents are then
recovered in the regenerator and recycled back and fed to the absorber. High
concentration of carbon dioxide is separated from the chemical solvents and directed to
next storage location.

Figure 1 Schematic diagram of carbon dioxide absorption and regeneration system

The use of monoethanolamine (MEA) in the carbon dioxide is limited due to some issues,
such as high heat of absorption and corrosion issues. On the other hand, the use of
potassium carbonate is also limited by the rate of absorption. Somehow, introducing of
promoters in the potassium carbonate solvent will increase the operation cost. The
advantages of using ammonia solution include high carbon dioxide absorption rates, high
carbon dioxide removal rates and also high carbon dioxide loading. The loss of ammonia
solution in the adsorption and desorption process is considered acceptable in terms of
124 U.K. Ghosh and S.C. Yee

environment as well as operating perspective (Dave et al., 2006). Yet, more researches
are needed because the absorption rate of carbon dioxide in ammonia solution is
infrequently researched. Thus, the paper will focus reaction kinetics of absorption and
equilibrium of carbon dioxide into aqueous ammonia.
In this research, the absorption of carbon dioxide into aqueous ammonia is studied. A
mathematical model is developed based on the mass balance of carbon dioxide
absorption. Besides that, the model is simulated in order to observe the absorption rate
with operational parameters. Finally, the simulated result is compared with literature data.

2 Solvents for carbon dioxide capture

The following are the criteria for selection of chemical solvents for carbon dioxide
absorption (Dutta, 2007):
a Solubility – The ideal chemical solution will only dissolve desired components, in
this case carbon dioxide, but should not dissolve other undesired components.
However, some undesired components also dissolve in the solvents. Thus, selectivity
of the right solvent is important in order to dissolve the desired product and also to
minimise the absorption of undesired products.
b Volatility – The selected solvent should have low volatility in order to prevent losses
of solvent during the process.
c Viscosity – The selected solvent should have low viscosity so that it can flow easily
during the process; especially operate in a packed column.
d Corrosiveness – The selected solvent should have no or limited corrosiveness, thus
lower cost of maintenance to the equipment is needed.

2.1 MEA as solvent

Mores et al. (2011) has investigated the modelling and optimisation of the chemical
absorption process in removing carbon dioxide by using MEA solutions. They had
considered the ratio between total absorbed carbon dioxide and the total cooling and
heating utilities, and the ratio between total absorbed carbon dioxide and the total amine
flow rates. Optimisation variables such as temperature, composition and flow rates of the
aqueous solution as well as the reboiler and condenser duties are considered in the
investigation.
The chemical reactions involved in the process are listed as below (Mores et al.,
2011):
2H 2O + CO2 ↔ H 3O + + HCO3− (1)

H 2O + HCO3− ↔ H 3O + + CO32− (2)

H 2O + MEAH + ↔ H 3O + + MEA (3)

MEAH + HCO3− ↔ H 2O + MEACOO − (4)

 Modelling and simulation of reaction kinetics of carbon dioxide absorption 125

MEA + CO2 + H 2O ↔ MEACOO − + H 3O + (5)

CO2 + OH − ↔ HCO3− (6)

MEA shows high capacity of carbon dioxide absorption; however, concerns such as high
operating condition, high heat of generation as well as corrosive properties of MEA
limited its application in practical plants.

2.2 Potassium carbonate (K2CO3) as solvent

As compare to MEA, potassium carbonate has lower solvent costs and requires lower
heat of regeneration of solvent. Conversely, the absorption of carbon dioxide by
potassium carbonate is relatively slow and thus, promoters are needed in the absorption
process in order to increase the rate of carbon dioxide absorption.
Cullinane and Rochelle (2004) had developed a model in order to investigate the
effect of aqueous potassium carbonate in the carbon dioxide absorption promoted by
piperazine in wetted-wall column. In the investigation, 0.6M of piperazine was added to
20–30% of potassium carbonate at the temperature range of 40–80°C. A significant
decrease of intermediate carbon dioxide loading, e.g., 85%, was shown by the addition of
0.6M promoter. The rate of absorption has been increased by 200% as the temperature
increases from 40–80°C. At high loading, a significant amount of piperazine dicarbamete
was formed while the piperazine carbamate remains unchanged. However, the absorption
did occur at low loading.
On the other hand, Ghosh et al. (2009) had done an experiment to study the
absorption rate of carbon dioxide into aqueous potassium carbonate promoted by boric
acid. In the experiment, the absorption rates of carbon dioxide in a wetted-wall column
were measured with and without 30% potassium carbonate and 1–5% of boric acid at the
temperature of 40–80°C. The addition of increasing of small amount of boric acid
resulted a significant increase in the rate of absorption by factor of 2. As the temperature
increased from 40–80°C in 30% potassium carbonate and 1% of boric acid, the
absorption rate has increased by a factor of approximately 2.
The chemical reactions involved in the process are listed as below (Cullinane and
Rochelle, 2004):
CO2( gas ) ↔ CO2( aq ) (7)

CO2( aq ) + 2H 2O ↔ HCO3− + H 3O+ (8)

HCO3− + H 2O ↔ CO32− + H 3O + (9)

2H 2O ↔ H 3O+ + OH − (10)

PZ + H 2O + CO2( aq) ↔ PZCOO− + H3O+ (11)

PZH + + H 2O ↔ PZ − + H 3O + (12)

PZCOO− + H 2O + CO2( aq ) ↔ PZ (COO − )2 + H 3O+ (13)

126 U.K. Ghosh and S.C. Yee

H + PZCOO − + H 2O ↔ PZCOO − + H 3O + (14)

2.3 Aqueous ammonia as solvent

Aqueous ammonia can be used to capture carbon dioxide by absorption process. Qin
et al. (2010) measured the kinetics of CO2 absorption in unloaded aqueous ammonia
solution by using a string of discs contactor. They found out that the kinetics rate constant
for CO2 absorption in ammonia solution was around 10% compared to other amines.
The chemical reactions involved in the process are listed as below:
CO2 + 2 NH3 ↔ NH 2COONH 4 (15)

CO2 + 2 NH 3 ↔ NH 2COO − + NH 4+ (16)

According to zwitterion mechanism, carbon dioxide reacts with ammonia to form

zwitterions. The zwitterions form in reaction [equation (17)] is involved in the second
reaction (18) in the presence of B, which is ammonia and water (NH3 and H2O) (Derks
and Versteeg, 2009):
K B , k2
CO2 + 2 NH 3 ←⎯⎯→ NH 2COO − + NH 4+ (17)

NH 3+ COO − + B ↔ NH 2COO − + BH + (18)

The overall rate equation is represented as below (Qin et al., 2010):

[CO2 ][ NH 3 ]
RCO2 − NH3 = (19)
1 k−1 1
+
k2 k2 ∑k B [ B]

Ammonia and water are considered the dominant based in aqueous ammonia. Therefore,
the overall rate equation is modified into equation (20) (Qin et al., 2010).
[CO2 ][ NH 3 ]
RCO2 − NH3 = (20)
1 1
+ Z
k2 k NH 3
[ NH 3 ] + kHZ 2O [ H 2O]

k2 k NH3
Z
k NH = (21)
3
k−1

k2 k H 2 O
k HZ 2O = (22)
k−1
where
k2 = forward reaction constant (m3.kmol.s–1)
[CO2] = concentration of CO2 (mol.m–3)
[NH3] = concentration of NH3 (mol.m–3)
[H2O] = concentration of H2O (mol.m–3)
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 127

RCO2 − NH 3 = reaction rate (kmol.m–3s–1)

k–1 = backward reaction rate constant.

For zwitterion mechanism,

⎛ −9062.0 ⎞
k2 = 1.7809 x1023 exp ⎜ ⎟ (23)
⎝ T ⎠
⎛ −4451.4 ⎞
Z
k NH = 3.9376 x108 exp ⎜ ⎟ (24)
⎝ T ⎠
3

⎛ −303.08 ⎞
kHZ 2O = 47.002exp ⎜ ⎟ (25)
⎝ T ⎠
where
T = operating temperature (K).

3 Theory of wetted wall column (WWC)

Wetted wall column is a classical experimental model set up for the investigation of the
absorption rate of carbon dioxide. The wetted wall column is made up of two vertical
cylinders, where the smaller cylinder is installed inside the other cylinder. The gas stream
containing carbon dioxide is flowing upwards through the annular space while the
solvent, aqueous ammonia is flowing in the opposite direction forming a film on the outer
wall of the inner tube. Absorption of carbon dioxide happens when the gas and liquid
streams contact with each others. The details of WWC can be found elsewhere (Ghosh
et al., 2009).

Figure 2 Schematic diagram of a wetted wall column (see online version for colours)

Liquid stream
Gas stream
128 U.K. Ghosh and S.C. Yee

3.1 Film theory for absorption accompanied by reaction

The motion of liquid ammonia can be assumed to be laminar when the liquid flows near
the wall. The concentration of dissolved carbon dioxide will decrease from CCO2 ,i at the
CO2-liquid ammonia interface to CCO2 ,b at the liquid bulk. The film theory is based on
the following assumptions (Dutta, 2007): The carbon dioxide transfer through the film is
at steady state conditions. No carbon dioxide will be accumulated in the system. Carbon
dioxide transfers through the stagnant fluid layer at the phase boundary.
In the mass balance, the rate of consumption of carbon dioxide by reaction must be
taken into consideration. Since the film theory occurs in a steady state condition, the mass
balance is written as below:
NCO2 |z − NCO2 |z + Δz = (Δ z )( RCO2 − NH3 ) (26)

where NCO2 |z is CO2 flux at point z. The flux is written in (27):

dCCO2
NCO2 = − DCO2 (27)
dz
Dividing the mass balance by ∆z and putting the limit ∆z → 0, and substituting the flux,
d 2CCO2
DCO2 = RCO2 − NH3 (28)
dz 2
where
CCO2 = CCO2 ,i at z = 0, (concentration of CO2 at gas-liquid interface)

CCO2 = CCO2 ,b at z = δ, (concentration of CO2 at the bulk liquid).

4 Mathematical model development

Material balance in term of CO2:

In − Out + Generation − Consumption = Accumulation (29)

Assumption:
No CO2 is generated in the system (generation = 0)
Steady-state system. In a absorption system, no accumulation happens in the system
(Accumulation = 0).
Thus, the material balance of CO2 is simplified into:
In − Out = Consumption (30)

( Fg CCO2 , g + FS CCO2 , S ) − ( Fg/ C CO

/
2 ,g
+ FS/ C CO
/
2 ,S
) = RCO2 − NH 3 V (31)
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 129

where
Fg = flow rate of gas stream entering the system (m3.s–1)
FS = flow rate of solvent stream entering the system (m3.s–1)

Fg/ = flow rate of gas stream leaving the system (m3.s–1)

FS/ = flow rate of solvent stream leaving the system (m3.s–1)

CCO2 , g = concentration of CO2 in the gas stream entering the system (mol.m–3)

CCO2 , S = concentration of CO2 in the solvent stream entering the system (mol.m–3)

/
C CO = concentration of CO2 in the gas stream leaving the system (mol.m–3)
2 ,g

/
C CO = concentration of CO2 in the solvent stream leaving the system (mol.m–3)
2 ,S

RCO2 − NH 3 = overall rate of reaction between ammonia and CO2 (mol.m–3.s–1)

V = volume of the solvent in the system (m3).

In the absorption system, ammonia solution is chosen as the solvent used to absorb CO2
in the gas stream. Initially, the ammonia solution stream contains no CO2, which the
concentration of CO2 in the solvent stream entering the system is equal to zero
( CCO2 , S = 0 ) . The reaction between CO2 and ammonia is assumed to follow the
zwitterion mechanism. In the reaction, ammonia and CO2 are reacted and form
zwitterion, where zwitterion is further deprotonated by a base (B) (Qin et al., 2010). The
overall rate of equation between NH3 and CO2 is represented by equation (20).
Since the CO2 is reacted and forms ammonium compound when leaving the system,
therefore, the concentration of CO2 leaving the system will be zero ( CCO
′ 2 , S = 0 ) . Thus,
the material balance of CO2 is further simplified into:

Fg CCO2 , g − Fg/ C CO
/
2 ,g
= RCO2 − NH 3 V (32)

In this system, the effect of temperature on the rate of absorption is tested at the operating
pressure of 1.4 bar. Two different operating temperatures, 293 K and 313 K (20°C and
40°C) were chosen in order to observe the effects. The overall rate of reaction for two
temperatures is calculated by using equations (23) to (25) (Qin et al., 2010). Both gas and
solvent flow rates are 5 SLPM and 2 × 106 m3/s respectively. The gas flow rate of
5 SLPM is converted into gas flow rates at 293 K and 313 K at pressure of 1.4 bar. At
standard condition, the temperature and pressure for gas are 273 K and 1.01325 bar or
101325 Pa, respectively. The gas flow rate is calculated from:

PV
1 1 PV
= 2 2 (33)
n1 RT1 n2 RT2
130 U.K. Ghosh and S.C. Yee

Since n1 = n2, the equation is simplified into:

PV
1 1 PV
= 2 2 (34)
T1 T2
Therefore, the gas flow rate at 313 K is 6.915 × 10–S ms–1.
The outlet partial pressure for CO2 in the gas stream is calculated from the material
balance. The temperature and the flow rates of inlet and outlet of gas stream is assumed
to be the same.

Fg (CCO2 , g − CCO
/
2 ,g
) = RCO 2 − NH 3V
(35)
Since,
n P
C= = (36)
V RT
Equation (36) is modified into:
Fg
( PCO2 , g − PCO
/
2 ,g
) = RCO2 − NH3 V (37)
RT
where
PCO2 , g = partial pressure of CO2 in the inlet of gas stream (kPa)

/
PCO 2 ,g
= partial pressure of CO2 in the outlet of gas stream (kPa).

In order to calculate the overall gas transfer coefficient, KG, the log mean pressure need to
be determined as the overall gas transfer coefficient, KG, is calculated as the slope of flux
versus log mean pressure (Liu et al., 2009).
PCO2 − PCO
/
Log mean pressure, PCO2 ,b = 2
(38)
⎛P 2 ⎞
Ln ⎜ CO ⎟⎟
⎜ P/
⎝ CO2 ⎠
where
PCO2 ,b = log mean pressure (kPa)

PCO2 = partial pressure of CO2 in the inlet of gas stream (kPa)

/
PCO 2
= partial pressure of CO2 in the outlet of gas stream (kPa).

The flux of CO2 is the number of moles of CO2 travel into and out of the solution. Thus,
the flux is calculated as below (Liu et al., 2009):
Fg
NCO2 = ( PCO2 , g − PCO
/
2 ,g
) (39)
RT
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 131

where
N CO2 = CO2 flux, number of moles of CO2 absorbed per second per unit area, moles
m2s1.
The overall gas transfer coefficient, KG, is calculated as the slope of flux to the log mean
pressure (Liu et al., 2009).
NCO2
KG = (40)
PCO2 ,b
where
KG = overall gas transfer coefficient (mol.pa–1.cm–2.s–1).

5 Simulation of mathematical model

The developed model is simulated using six cases:

Case 1 10% CO2 contact with 1%, 5%, 10% and 15% NH3 at 293 K
Case 2 10% CO2 contact with 1%, 5% and10% NH3 at 313 K
Case 3 10% NH3 contact with 5%, 10%, 15% and 20% CO2 at 293 K
Case 4 10% NH3 contact with 5%, 10%, 15% and 20% CO2 at 313 K
Case 5 Effect of different height to 10% CO2 contact with 1%, 5% and 10% NH3 at
293 K
Case 6 Effect of different height to 10% CO2 contact with 1%, 5% and 10% NH3 at
313 K.
The results obtained from simulation based on Case 1 to Case 4 will be compared with
the experimental results obtained from (Liu et al., 2009; Qin et al., 2010). Further results
discussion will be presented on results and discussion.

6 Results and discussion

For Case 1, 10% of inlet concentration of CO2 is contacted with 1%, 5% and 10%
ammonia solution at operating temperature of 293 K. For Case 2, 10% of inlet
concentration of CO2 is contacted with 1%, 5%, 10% and 15% ammonia solution at
operating temperature of 313 K. Higher ammonia solution concentrations show better
absorption rate in both case (Figure 3). 15% ammonia solution shows better absorption
rate than other ammonia solution concentration at operating temperature of 293 K. 10%
ammonia solution shows better absorption rate than other ammonia solution
concentration at operating temperature of 313 K. The reaction rate between CO2 and
ammonia solution is highly depended on the concentration of ammonia solution.
132 U.K. Ghosh and S.C. Yee

However, experiment conducted by Liu et al. (2009) shows that the concentration of
ammonia solution should be selected in the range from 5%–10%. The use of higher
concentration of ammonia solution in practical may faced issues such as volatility of
solution (Qin et al., 2010). As mention by Cullinane and Rochelle (2004), increase of
temperature from 40°C to 80°C increase the rate of CO2 absorption by promoted K2CO3
solution by a factor of two at a constant CO2 vapour pressure. Yet, the effect of
temperature was not obvious from the result (Figure 3). The ammonia solution is believed
to be evaporated at a higher temperature.

Figure 3 Flux for absorption of CO2 into different concentration of ammonia solution (see online
version for colours)

For both Case 3 and Case 4, 10% concentration of ammonia solution is contacted with
5%, 10%, 15% and 20% CO2 at operating temperature of 293 K and 313 K respectively
(Figure 4). Higher concentration of CO2 in the inlet gas stream shows better absorption
rate in both operating temperatures. Higher concentration of CO2 in the inlet gas stream,
increase the concentration gradient between two streams which leads to higher absorption
rate of CO2. However, the effect of temperature was not obvious from the result
(Figure 4). This phenomenon is similar to the results shown in Figure 3.
The overall gas transfer coefficient, KG is calculated from equations (38) and (39).
The KG lines at 293 K in 1%, 5%, 10% and 15% ammonia solution is plotted and shown
in Figure 5, while the KG lines at 313 K in 1%, 5% and 10% ammonia solution is plotted
and shown in Figure 6. The KG lines at 293 K in 5%, 10%, 15% and 20% CO2 inlet
concentration is plotted and shown in Figure 7, while the KG lines at 313 K in 5%, 10%,
15% and 20% CO2 inlet concentration is plotted and shown in Figure 8. By assuming KG
lines are linear, the plotted lines are used to predict the CO2 flux at different temperatures
and concentration of ammonia solutions as well as different CO2 inlet concentration. At
the same temperature, the CO2 flux increases with the concentration of ammonia solution.
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 133

Figure 4 Flux for absorption of CO2 into different concentration of CO2 inlet (see online version
for colours)

Figure 5 Flux CO2 partial pressure lines by calculated KG at 293 K – promoted by different
concentration of NH3(aq) (see online version for colours)

KG = KG × 1010(mol/pa.cm2.s)
134 U.K. Ghosh and S.C. Yee

Figure 6 Flux CO2 partial pressure lines by calculated KG at 313 K – promoted by different
concentration of NH3 (aq) (see online version for colours)

KG = KG × 1010(mol/pa.cm2.s)

Figure 7 Flux CO2 partial pressure lines by calculated KG at 293 K – promoted by different inlet
concentration of CO2 (see online version for colours)

KG = KG × 1010(mol/pa.cm2.s)
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 135

Figure 8 Flux CO2 partial pressure lines by calculated KG at 313 K – promoted by different inlet
concentration of CO2 (see online version for colours)

KG = KG × 1010(mol/pa.cm2.s)

For both Case 5 and Case 6, the effect of column heights is tested on 10% concentration
of ammonia solution contacted with 5%, 10%, 15% and 20% CO2 at operating
temperature of 293 K and 313 K. The absorption rates of CO2 are highly dependent on
the contact area during the process. However, increase of contact area or column height
may increase the pressure drops in the column, which caused large effects on the CO2
flux across two streams (Mores et al., 2011). As the pressure drop increases the driving
force for CO2 separation decreases and hence the CO2 flux decreases.

Figure 9 Effect of column heights to the CO2 flux with different concentration of ammonia
solution at 293K (see online version for colours)
136 U.K. Ghosh and S.C. Yee

Figure 10 Effect of column heights to the CO2 flux with different concentration of ammonia
solution at 313 K (see online version for colours)

The modelling results are compared with experimental results by Liu et al. (2009) and
tabulated in Table 1 to Table 4. However, the modelling results are different from the
experiment results obtained by Liu et al. (2009). There are some factors that will cause
the difference of both results. During the experiment, random errors are encountered
during the measurement as disturbances may occur when the readings are taken. The
supply of gas stream may be not consistent, which leads to fluctuation of CO2 partial
pressure readings. Besides that, the operating temperature may vary as heat is transferred
to the environment during practical.
In term of modelling, assumptions which have been made previously may cause
errors of modelling results. During modelling, the inlet and outlet gas flow rates are
assumed to be the same and this may cause the deviation between the experimental and
modelling results. On the other hand, the modelling methodology is considered ideal and
may be impractical to implement into real world.

Table 1 Comparing simulated results with literature data for Case 1

KG (mol/pa.cm2.s) KG (mol/pa.cm2.s)
T (K) NH3 Concentrations (%)
experiment results modelling results
293 1 0.243 × 10–10 0.022 × 10–10
293 5 0.698 × 10–10 0.111 × 10–10
293 10 0.978 × 10–10 0.225 × 10–10
293 15 1.392 × 10–10 0.341 × 10–10
 Modelling and simulation of reaction kinetics of carbon dioxide absorption 137

Table 2 Comparing simulated results with literature data for Case 2

KG (mol/pa.cm2.s) KG (mol/pa.cm2.s)
T (K) NH3 Concentrations (%)
experiment results modelling results
313 1 0.351 × 10–10 0.022 × 10–10
313 5 1.191 × 10–10 0.111 × 10–10
–10
313 10 1.644 × 10 0.228 × 10–10

Table 3 Comparing simulated results with literature data for Case 3

KG (mol/pa.cm2.s) KG (mol/pa.cm2.s)
T (K) CO2 Concentrations (%)
experiment results modelling results
293 5 1.054 × 10–10 0.280 × 10–10
293 10 0.978 × 10–10 0.225 × 10–10
–10
293 15 0.971 × 10 0.215 × 10–10
293 20 1.103 × 10–10 0.209 × 10–10

Table 4 Comparing simulated results with literature data for Case 4

KG (mol/pa.cm2.s) KG (mol/pa.cm2.s)
T (K) CO2 Concentrations (%)
experiment results modelling results
313 5 1.743 × 10–10 0.282 × 10–10
–10
313 10 1.644 × 10 0.228 × 10–10
313 15 1.507 × 10–10 0.215 × 10–10
313 20 1.607 × 10–10 0.209 × 10–10

7 Conclusions

In this paper, a mathematical model for the reaction kinetics of carbon dioxide absorption
into aqueous ammonia in a wetted wall column is developed. Simulation of the
mathematical model is performed and the simulated results are compared with literature
data. Higher ammonia solution concentrations show better absorption rate, and yet, the
use of higher concentration of ammonia solution in practical may faced issues such as
volatility of solution. Liu et al. (2009) suggested that the concentration of ammonia
solution should be selected among 5%–10%. Higher concentrations of CO2 in the inlet
gas stream show better absorption rate in both operating temperature. However, the effect
of temperature was not obvious from the modelling results obtained. By assuming KG
lines are linear, the plotted lines are used to predict the CO2 flux at different temperatures
and concentration of ammonia solutions as well as different CO2 inlet concentration. At
the same temperature, the CO2 flux increases with the concentration of ammonia solution.
The absorption rates of CO2 are highly dependent on the contact area during the process.
However, increase of contact area or column height may increase the pressure drop in the
column, which causes large effects on the CO2 flux across two streams.
138 U.K. Ghosh and S.C. Yee

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