Computers and Chemical Engineering 53 (2013) 178–189

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Computers and Chemical Engineering

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

Dynamic modelling of the absorber of a post-combustion CO2 capture

plant: Modelling and simulations
Sanoja A. Jayarathna a , Bernt Lie a , Morten C. Melaaen a,b,∗
a
Faculty of Technology, Telemark University College, Porsgrunn, Norway
b
Tel-Tek, Porsgrunn, Norway

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

Article history: Modelling work related to carbon dioxide (CO2 ) capture technologies is of great importance with respect
Received 28 May 2012 to the design, control, and optimization of the capture process. Development of dynamic models as such is
Received in revised form 23 January 2013 important since there is much information embedded with the dynamics of a plant which cannot be stud-
Accepted 3 March 2013
ied with steady state models. A model for the absorption column of a post-combustion CO2 capture plant
Available online 13 March 2013
is developed following the rate based approach to represent heat and mass transfer. The Kent–Eisenberg
model is used to compute the transfer and generation rates of the species. Sensitivity of the model for
Keywords:
different physiochemical property correlations is analyzed. The predictions of the dynamic model for the
CO2 capture
Dynamic model
capture plant start-up scenario and operation of the absorption column under varying operating condi-
Absorption tions in the up-stream power plant and the down-stream stripping column are presented. Predictions
MATLAB of the transient behaviour of the developed absorber model appear realistic and comply with standard
steady state models.
© 2013 Elsevier Ltd. All rights reserved.

1. Introduction
Power generation via fossil fuel-fired power plants is known
to be the largest single source of CO2 emission (Freund, 2003). The
development of capture technologies targeting such sources there-
fore is important for achieving the goals in CO2 emission reduction.
Post-combustion capture, pre-combustion capture and oxy-fuel
combustion are the three main technologies available at present
(Cormos, Gasper, Padurean, & Cormos, 2010), and much research
is done with the prospect of developing those techniques further.
Post-combustion capture is still the best known technique, possibly
due to the large number of existing power plants, and the promising
developments that are available. CO2 capture by amine absorption
and stripping is currently considered to be the most feasible option
for the removal of carbon dioxide from the power plants’ exhaust
gases (Plaza, Wagener, & Rochelle, 2009).
A process flow diagram of an amine based capture plant is given
in Fig. 1. The exhaust gas stream from the power plant, which enters
at the bottom of the absorption tower, flows counter currently with
an amine stream to which the CO2 is transferred, before leaving as
a cleaned gas stream from the top of the tower. The amine stream
leaving the absorption tower with absorbed CO2 is treated in the
∗ Corresponding author at: Faculty of Technology, Telemark University College,
Kjølnes ring 56, P.O. Box 203, N 3901 Porsgrunn, Norway. Tel.: +47 35575286;
fax: +47 35575001.
E-mail address: morten.c.melaaen@hit.no (M.C. Melaaen).
stripping tower by removing the CO2 with the use of steam, and is
then recycled.
Modelling work related to CO2 capture via amine absorption
plays an important role with respect to the design, control and opti-
mization of the capture process. Several steady state models are
already in use for design and optimization purposes, but dynamic
simulation models are scarce. Development of dynamic models is
important since there is much information related to the dynamics
of a plant, such as the transient conditions during the start-up and
shut-down and the operation of the plant under varying loads.
A CO2 capture plant with solvent absorption (absorber/stripper
process) consists of several units which will interact and eventually
influence the control and optimization of the process. The operation
of a power plant always depends on the power demand and avail-
ability of other utilities which can lead to variations in its load. The
load variations in the up-stream power plant cause varying exhaust
gas rates which may cause operating challenges for the CO2 capture
plant. A dynamic simulation model should predict the influence
of the components of the capture plant on each other. Further,
the model should predict the influence from the up-stream power
plant on the operation of the capture plant, when the power plant
is running under varying load conditions. In addition, the need of a
dynamic model for simulation becomes vital as the complexity of
the process increases due to the advancements in technology. Use of
pinch technology and heat integration, and multi pressure configu-
ration have already been proposed by researchers and exemplifies
the advancement of the technology (Harkin, Hoadley, & Hooper,
2010; Oyenekan & Rochelle, 2006).

0098-1354/$ – see front matter © 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.compchemeng.2013.03.002
 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189 179

Further, heat and mass transfer are actually rate based processes
Nomenclature that are driven by the gradients of temperature and chemical poten-
tials. In the NEQ approach, the finite mass transfer rates across
Aw inter-phase contact area (m2 /m3 ) the liquid–vapour interface are considered. The NEQ approach has
AT effective area for heat loss (m2 ) been introduced in steady state simulators like Aspen Plus (Tönnies,
C̃pl molar specific heat capacity (J/mol K) Mangalapally, & Hasse, 2011) and is even more appropriate for
Ĉpl mass specific heat capacity (J/g ◦ C) dynamic models.
CO2 carbon dioxide The dynamic models developed for representing industrial
c concentration (mol/m3 ) absorption processes have to be accurate and rigorous in order
E enhancement factor to give insight in the complex transient conditions, and simple to
Hab , Hvap heat of absorption, heat of vaporization (nega- ensure the feasibility of the process simulations (Schneider, Sander,
tive value) (J/K) & Górak, 2003). Simplicity will ensure higher execution speed,
H Henry’s law coefficient which is an important factor since simulation of transient condi-
hL liquid hold-up (liquid volume/total volume) tions is much more complex than steady state simulations. Further,
hov , hout heat transfer coefficient (between phases, wall) to be used in advanced control applications (e.g. MPC), the model
(J/m2 K) must be solvable in fractions of real-time; this is not possible with
k, kov mass transfer coefficient (local, overall) (m/s) a complex model. Therefore, it is important to make the model
MEA monoethanolamine as simple as possible yet good enough to be used in a dynamic
MEACOO− carbamate ion of MEA simulator. Use of simple thermodynamics can be considered as a
MEAH+ protonated MEA wise strategy for developing a dynamic model to ensure simplic-
 
ṅt , ṅg volumetric molar rate (inter-phase transfer, gener- ity. The Kent–Eisenberg model (Kent & Eisenberg, 1976) is such a
ation) (mol/m3 s) simple model while the e-NRTL model (Hessen, Haug-Warberg, &
T temperature (K) Svendsen, 2010) would be a complex model. Use of models like
t time (S) e-NRTL is important in steady state models used for tasks such
u velocity (m/s) as equipment design, where more accurate thermodynamics is
z packing height (m) needed.
Validation of the predictions of the dynamic model still remains
Greek symbols a challenge due to the absence of appropriate experimental data.
 density (kg/m3 ) Comparing the predicted steady states from such a dynamic model
with the experimental data available in the literature is a possible
Symbols first step in validating the model.
* hypothetical equilibrium state value Little work exists on the development of dynamic models of
the absorption tower of a post-combustion CO2 capture plant
Superscripts (Biliyok, Lawal, Wang, & Seibert, 2012; Jayarathna, Lie, & Melaaen,
l liquid phase 2011; Kvamsdal, Jakobsen, & Hoff, 2009; Lawal, Wang, Stephenson,
v vapour phase Koumpouras, & Yeung, 2010; Lawal, Wang, Stephenson, & Yeung,
2009). The majority of the existing models have used complex ther-
modynamic models which increases the complexity of the models.
In recent years, the popularity of the non-equilibrium rate Biliyok et al. (2012) have validated their model using a set of
based approach (NEQ) for column modelling has surpassed that dynamic data. Validation of the rest of the developed models is
of the equilibrium stage approach (EQ), where the liquid and performed by comparing the predictions of the CO2 removal effi-
vapour phases are assumed to be in equilibrium. The EQ stage ciencies and the column temperature profiles at the steady state
and efficiency based approaches are not very accurate because with the literature data. The Pilot Plant Cases from the Separations
columns rarely, if ever, operate at equilibrium in actual operation. Research Program at the University of Texas at Austin are used

Condenser
Cleaned Gas
Buffer Tank Amine
Cooler CO2
Reflux to the
Drum compressor

Reflux
Stream
P/P heat
exchanger

Stripping
Absorption Column
Column
Exhaust from Re-boiler
the Power Plant
Rich Amine Lean Amine

Fig. 1. An amine based CO2 capture plant.

180 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189

as the literature data (Dugas, 2006; Kvamsdal & Rochelle, 2008). from the liquid phase and included in the liquid phase energy
The flue gas rate and/or the packing height of the column used in balance.
the simulations of the majority of the previous work are different
from those of the Pilot Plant Cases. The alterations of the pack- 3.1. Main model equations
ing height or the gas flow rate are introduced in order to get the
predictions within the range of the Pilot Plant data, as the model The main model equations are developed by applying the com-
predictions are not very good otherwise. A possible reason for this ponent and energy balances for the liquid and vapour phases,
is the under-predictive or over-predictive tendency of the used cor- respectively. The balance between the molar flow into a control
relations and models (e.g. model proposed by Onda, Takeuchi, and volume (CV), flow out from a CV, generation and inter-phase trans-
Okumoto (1968) for wetted specific area, Aw ) for the prediction of fer in a CV for specie “i” in each phase is considered in the specie
the packing properties. Further, most of the models developed ear- balance. Reactions in the vapour phase are neglected. The specie
lier have considered the transfer of CO2 only or CO2 and H2 O from balances lead to Eqs. (1) and (2):
one phase to the other, which may also have affected the model
predictions. ∂cil l
ul ∂ci 1 
= + ṅ + ṅ (1)
∂t hL ∂z hL i,t i,g

2. Novelty of the work ∂civ uv ∂civ 1

=− − ṅ (2)
∂t (1 − hL ) ∂z (1 − hL )
This paper presents an improved version of the dynamic model
presented by Jayarathna et al. (2011), which is developed for an Rate of change of concentration of specie “i” in the liquid and
absorption tower of a MEA (Mono-Ethanol-Amine) based CO2 cap- vapour phase are given by Eqs. (1) and (2), respectively.
ture plant. Better representation of the interfacial mass transfer, The balance between the energy flows into a control volume
physical properties of the amine solution and packing hydraulics (CV), flow out from a CV, and heat added to a CV for each phase
are introduced in the improved model. The sensitivity of the model is considered in the energy balance. The energy balances lead to
for different physiochemical correlations is analyzed. The effect on Eqs. (3) and (4) which describe the rate of change of liquid tem-
the predictions of the model from the inclusion of minor reactions perature and vapour temperature inside the absorption column,
(presented by Kent and Eisenberg, 1976) in addition to the main respectively.
reaction between MEA and CO2 , and transfer of minor species is
∂T l ul ∂T l hov Aw
also analyzed. = +  l (T v − T l )
∂t hL ∂z hL Ĉpl (c Mwi )
The predictions of the model for the plant start-up scenario and i i
the operation under varying load conditions from the up-stream 
hout AT ṅCO
power plant and the down-stream stripping column are included. l amb
−  (T − T )+  2,t
(−H̃ab )
The model has been developed following the NEQ approach and hL Ĉpl (c l Mwi )
i i
hL Ĉpl (c l Mwi )
i i
using the Kent–Eisenberg (K–E) model, which is a simple concen-
tration based model, to compute the driving forces of the reaction
 
ṅi,t
+  (−H̃vap,i ) (3)
and mass transfer rates. The model is implemented in MATLAB and hL Ĉpl i
(cil Mwi )
i
the solver ode15s is used for performing the simulations.
The model presented in this paper has a simple and clear rep-
resentation of the physics and thermodynamics of the absorption ∂T v uv ∂T v hov Aw
process. Specifically, the use of the K–E model, which is a simple
=− −  (T v − T l ) (4)
∂t (1 − hL ) ∂z (1 − hL ) (civ C̃pv )
concentration based and well documented model with few param-
i
eters, makes it easy to reproduce the tower model without much
effort. Therefore, the easy adoptability and transparency makes this The MEA solvent system is considered for the analysis, and the
work interesting for the researchers in the field. thermodynamic and physical parameters are given accordingly.

3.2. Interfacial mass transfer

3. Dynamic model
The dynamic model development for the absorption column of
a MEA based CO2 capture plant and the model equations have been
published by Jayarathna et al. (2011). The predictions of the model
for the steady state are compared with literature data and published
in the same work.
The model that was previously published is improved through
the introduction of the transfer of MEA. The model proposed by
Weiland, Dingman, Cronin, and Browning (1998) for calculating
the liquid phase density is included instead of the model pro-
posed by Cheng, Meisen, and Chakma (1996), which was used
in the previous version of the model. The wetted area of the
packing is represented using a correlation found in the litera-
ture which is specifically proposed for IMTP packing (IMTP40#
is used in the model, and the Pilot Plant Study) (Hanley & Chen,
2012). Further modification is the introduction of heat loss to the
surroundings with use of an average value for the heat trans-
fer coefficient of the column wall from the literature (Kvamsdal
et al., 2009). The heat loss to the surroundings is assumed to be
Transfer of N2 and O2 between the phases has been considered to
be negligible. CO2 , H2 O and MEA transfer is allowed for both direc-
tions between the phases, and the fluxes are given by the following
relation:
ṅ
i,t
v A (c v − c v∗ )
= ki,ov w i i
(5)
The concentrations at the hypothetical equilibrium state are
found using the saturation vapour pressure for H2 O and MEA, and
Henry’s law coefficient for CO2 . Correlations for saturation vapour
pressure for water and Henry’s law coefficient are given by Hoff
(2003) and the Kent–Eisenberg model (Kent & Eisenberg, 1976).
Saturation pressure of MEA is found by correlating the data found
in the literature (Chem Group, 2011).
The overall mass transfer coefficient represents the effect from
both the liquid side resistance and vapour side resistance on the
mass transfer. For H2 O and MEA the liquid side resistance is
assumed to be negligible, so that the overall mass transfer coeffi-
cient is replaced with the local gas side mass transfer coefficient. For
 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189 181

Table 1
Literature sources of some important physical properties.

Property Source Applicable range Comments

Enhancement factor Hoff (2003) 2 < E < 103

Forward reaction rate coefficient
Heat of absorption of CO2
Heat of vaporization of H2 O
Heat of vaporization of MEA
Liquid density
Liquid diffusivity of CO2
Liquid hold-up
Liquid viscosity
Mass transfer coefficients
Overall heat transfer coefficient
between phases
Phase and reaction equilibrium
Saturation pressure of water
Thermal conductivity of N2
Vapour diffusivity
Vapour viscosity
Wetted area of packing
Jamal et al. (2006) 293 ≤ T ≤ 383
Kohl and Nielsen (1997) 0 ≤ ˛ ≤ 1.2, 30 wt% MEA
a
Gaspar and Cormos (2011) Function of pressure
a
Gaspar and Cormos (2011) Function of temperature
Weiland et al. (1998) 298 ≤ T ≤ 398, 0 ≤ ˛ ≤ 0.6
Versteeg and Van Swaaij (1988) 273 ≤ T ≤ 353 N2 O analogy is used
Billet and Schultes (1999) uv ≤ uv,s
Reid, Prausnitz, and Sherwood (1977) Tr ≤ 0.75 Mixture viscosity is found by
combining the individual component
values using a log mixing rule
Onda et al. (1968) For random packing,
absorption, desorption and
distillation with 20–30% error
Cussler (2009) Fluid–fluid transfer, turbulent Chilton–Colburn analogy is used
flow
Kent and Eisenberg (1976) 298 ≤ T ≤ 413, 3.06 ≤ %wt Simple and easy to apply
MEA ≤ 58.1
Hoff (2003) *
Incropera, Dewitt, Bergman, and Lavine (2007) 250 ≤ T ≤ 400
Poling, Prausnitz, and O’Connell (2001) For dilute component i diffuse Fuller’s equation is used for binary gas
into a homogeneous mixture systems, Blanc’s law is used to find the
value for the mixture
Perry and Green (1999) and Themelis (1995) 250 ≤ T ≤ 600. For gas mixtures Mixture viscosity is found by
at low to moderate pressure combining the individual component
values
a
Hanley and Chen (2012) Specific for IMTP packing

uv,s = loading point velocity for a counter current flow.

a
Have been used in the literature for absorption modelling (Hanley & Chen, 2012; Hoff, 2003; Gaspar & Cormos, 2011).

CO2 the overall mass transfer coefficient is given by the following
relation:
v 1
kCO = (6)
2 ,ov v ) + (H l
(1/kCO CO2 /kCO E)
2 2
Here ki (i = CO2 ) is the local mass transfer coefficient, H is the Henry’s
law coefficient and E is the enhancement factor. The enhance-
ment factor is used in Eq. (6) in order to represent the effect from
the reactions on the mass transfer rate and the value is found
from the correlation presented by Hoff (2003). Local mass trans-
fer coefficients are calculated using the correlation presented by
Onda et al. (1968).
3.3. Reaction kinetics and phase equilibrium
The reaction kinetics is important for introducing the rate
of specie generation to the model and the phase equilibrium is
important for interfacial mass transfer. The equilibrium reaction
constants and the phase equilibrium are represented according to
the Kent–Eisenberg model (Kent & Eisenberg, 1976). The use of the
simple concentration based K–E model ensures the simplicity of
the column model and short execution time. Further, the few and
available parameters of the K–E model makes it easier to include in
modelling work compared to more complex models. Only the main
reaction between CO2 and MEA, which is given by reaction R1, is
considered for computing the rate of generation of species.
−
CO2 + 2MEA←→MEAH+ + MEACOO−
Here MEAH+ is the protonated MEA and MEACOO− is the carbamate
ion formed by the reaction. The forward reaction rate coefficient
is introduced as a correlation found from Jamal, Meisen, and Lim
(2006), while the equilibrium coefficient for the overall reaction
is found as a combination of the coefficients available with the
Kent–Eisenberg model.
3.4. Physical properties and other parameters
Physical properties and other parameters are introduced to the
model either as correlations or constant values found in the liter-
ature, or else using well-known calculation methods. Some of the
important physical property correlations and other parameters are
given in Table 1 with their literature sources.
3.5. Model validation
The developed model is validated against the available exper-
imental data for steady state operations. Dynamic validations are
not possible at this state of the work due to the absence of dynamic
data. Biliyok et al. (2012) have validated their model using dynamic
data, but their data are confidential and not available for this work.
Several pilot plant runs (nos: 28, 30, 32, 36, 40, 43, 45 and 47)
from the Separations Research Program at the University of Texas
at Austin (presented by Dugas, 2006; Zhang et al., 2009) are used
for the validation of the modified dynamic model. The absorption
column in the pilot plant is a packed column with a diameter of
0.427 m and the total packing height of 6.1 m. This column consists
of two 3.05 m packing sections with a collector plate and redistribu-
tors in between (Dugas, Rochell, & Seibert, 2006). Applied packing
properties are taken from the literature (Jayarathna et al., 2011).
Flow rates, CO2 mole fractions, lean CO2 loadings and inlet temper-
atures are given in Table 2. Mole fractions of H2 O and N2 are taken
as 0.013 and 0.7528, respectively, for all the cases. The mole frac-
(R1) tion of O2 was corrected according to the variations in the CO2 mole
fraction in the flue gas stream. The model predictions are satisfac-
tory, and details are given in Table 3. Temperature profiles inside
the column for the pilot plant runs 28, 32, 40 and 47 are given in
Fig. 2. The solid lines (—) and dash–dot lines (-.-.) represent the liq-
uid and vapour phase temperature profiles inside the absorption
tower at the steady state, respectively, and the markers represent
the experimental data.
182 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189

Table 2
Inputs and predictions for the Texas Pilot Plant Runs (Dugas, 2006; Zhang et al., 2009).

Run no. Inlet liquid temp [K] Inlet gas temp [K] Lean CO2 loading yCO2 Inlet liquid rate [m3 /s] Inlet gas rate [mol/s]

28 313 321 0.29 0.165 13.7 × 10−4 7.025

30 313 325 0.284 0.166 8.2 × 10−4 6.960
32 314 320 0.279 0.177 6.8 × 10−4 3.520
36 313 326 0.284 0.175 7.1 × 10−4 3.510
40 313 329 0.229 0.168 13.9 × 10−4 6.790
43 313 327 0.231 0.160 6.6 × 10−4 6.850
45 314 327 0.285 0.169 10.0 × 10−4 5.145
47 313 332 0.281 0.180 5.0 × 10−4 5.060

yCO2 , mole fraction of CO2 in the inlet gas.

Table 3 are given in Fig. 5 for the pilot plant run 47. The experimental data
Comparison of the model predictions with data from the literature (Zhang et al.,
(from pilot plant run 32 and 47) are also included in Figs. 3–5.
2009).
Cases 1 and 2 analyze the effect of using the correlations from
Run no. Rich CO2 loading CO2 removal % Onda et al. (1968) and Billet and Schultes (1999), respectively, for
Experimental Simulated Experimental Simulated predicting the wetted specific area of the packing. Onda’s correla-
tion and Billet’s correlation seam to be predicting lower wetted area
28 0.412 0.425 86 83
30 0.453 0.448 70 67 compared to the correlation from Hanley and Chen (2012), which
32 0.428 0.444 95 94 is used in the base case. Therefore, the predicted ˛rich and  values
36 0.425 0.442 95 96 are lower and the temperature bulge is smaller compared to the
40 0.371 0.371 94 90 base case simulations.
43 0.491 0.451 72 68
45 0.433 0.445 96 98
The correlation from Hanley and Chen (2012) (Case 3) predicts
47 0.539 0.471 69 54 lower values for the local mass transfer coefficients compared to
the correlation from Onda et al. (1968), which is used in the base
case. As a result, the gas phase temperature profile is predicted as a
4. Sensitivity analysis rather flat profile (very small changes in the gas phase temperature)
compared to the other cases. The gas side mass transfer coefficient
Sensitivity of the model for different physiochemical correla- has a direct effect on the overall heat transfer coefficient according
tions, inclusion or exclusion of some minor reactions compared to the Chilton–Colburn analogy (Cussler, 2009).
to main reaction R1 and transfer of other components such as N2 The predicted temperature bulge for the Case 4 simulations
and O2 between the phases is analyzed. The set of minor reactions (saturation pressure Psat of water computed with the Clausius
included in the work are taken from the Kent–Eisenberg model Clapeyron model (Elliott & Lira, 1998)) is considerably higher than
(Kent & Eisenberg, 1976). Nine different cases are simulated and the temperature bulge from the base case and the experimental
compared with the experimental data and the base case simula- data points (Figs. 3 and 5). The reason for this observation can be
tion results, in which the model is used as presented in this paper. the lower saturation pressure value of water predicted by the Clau-
Each case analyze the effect on the removal efficiency (), rich CO2 sius Clapeyron model compared to the correlation by Hoff (2003).
loading (˛rich ), and the prediction of the temperature inside the In this case, variable responses are observed related to ˛rich and .
tower, from each alteration to the base case. Some pilot plant runs (43 and 47) show an increase and the rest
Details of the cases with the alterations made, as well as pre- of the pilot plant runs show a decrease compared to the base case.
dicted  and ˛rich values are given in Tables 4 and 5. Comparison Pilot plant runs 43 and 47 are experiments with limited amount
of the temperature profiles from the base case simulation and nine of amine solution available compared to the CO2 inlet flow and
cases specified in Tables 4 and 5 are given in Figs. 3 and 4 for the the rest is with excess amine flow. Under-prediction of Psat for the
pilot plant run 32. Temperature profiles for several selected cases runs with excess solution may have reduced the H2 O vaporization

Table 4
Experimental data and predictions of the CO2 removal efficiency.

Case Amendment CO2 removal %

P.P. Case 28 P. P. Case 30 P. P. Case 32 P. P. Case 36 P. P. Case 43 P. P. Case 45 P. P. Case 47

Pilot plant data – 86 70 95 95 72 96 69

Base case – 83 67 94 96 68 97 54
Case 1 Wetted specific area from Onda et al. 75 65 90 90 65 94 52
(1968)
Case 2 Wetted specific area from Billet and 79 66 90 90 64 95 52
Schultes (1999)
Case 3 Mass transfer coefficients from Hanley 81 71 94 94 68 97 55
and Chen (2012)
Case 4 Saturation pressure of water from 83 65 90 94 71 97 56
Clausius Clapeyron model (Elliott &
Lira, 1998)
Case 5 Saturation pressure from Antoine 83 65 91 95 68 97 55
equation (Elliott & Lira, 1998)
Case 6 Liquid density from Cheng et al. (1996) 83 67 92 95 69 97 54
Case 7 CO2 and H2 O transfer 83 68 95 96 69 98 55
Case 8 CO2 , H2 O, MEA, N2 and O2 transfer 83 67 94 96 68 97 54
Case 9 All reactions included 84 73 97 96 73 98 62
 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189 183

Table 5
Experimental data and predictions of the rich CO2 loading.

Case Amendment Rich CO2 loading

P.P. Case 28 P. P. Case 30 P. P. Case 32 P. P. Case 36 P. P. Case 43 P. P. Case 45 P. P. Case 47

Pilot plant data – 0.412 0.453 0.428 0.425 0.491 0.433 0.539
Base case – 0.425 0.448 0.444 0.442 0.451 0.445 0.471
Case 1 Wetted specific area from Onda et al. 0.412 0.444 0.438 0.433 0.443 0.439 0.466
(1968)
Case 2 Wetted specific area from Billet and 0.419 0.444 0.437 0.432 0.441 0.441 0.465
Schultes (1999)
Case 3 Mass transfer coefficients from Hanley 0.422 0.456 0.445 0.439 0.450 0.444 0.473
and Chen (2012)
Case 4 Saturation pressure of water from 0.425 0.444 0.437 0.440 0.460 0.445 0.478
Clausius Clapeyron model. (Elliott &
Lira, 1998)
Case 5 Saturation pressure from Antoine 0.425 0.442 0.439 0.441 0.453 0.445 0.474
equation (Elliott & Lira, 1998)
Case 6 Liquid density from Cheng et al. (1996) 0.425 0.447 0.441 0.440 0.454 0.445 0.472
Case 7 CO2 and H2 O transfer 0.422 0.445 0.442 0.439 0.448 0.442 0.469
Case 8 CO2 , H2 O, MEA, N2 and O2 transfer 0.425 0.448 0.444 0.442 0.451 0.445 0.471
Case 9 All reactions included 0.426 0.461 0.449 0.443 0.469 0.446 0.499

(a) 340 (b)

340
330
330
T [K]

320 T [K]
320

310 310
0 2 4 6 0 2 4 6
H, packing [m] H, packing [m]
(c) (d)
340 350

340
330
T [K]

T [K]

330
320
320

310 310
0 2 4 6 0 2 4 6
H, packing [m] H, packing [m]

Fig. 2. Comparison of the steady state results of the simulations with pilot plant data. – is liquid phase temperature, -.- is vapour phase temperature, * is experimental data.
(a) Pilot plant run 28, (b) Pilot plant run 32, (c) Pilot plant run 40 and (d) Pilot plant run 47.

significantly and then reduced the CO2 transfer, resulting in the
lower  and ˛rich values.
Observations related to the predictions from Case 5 are similar
to the observations from Case 4, which implies that Psat of water
computed by the Antoine equation is also lower compared to the
value in the base case.
The density model from Cheng et al. (1996) is used in the simu-
lations of Case 6. Density values predicted by Cheng’s model must
be lower compared to the values predicted by Weiland’s model
(Weiland et al., 1998) as the effect from the CO2 loading on the
solution density is not included. Reduced liquid density causes the
reduction of the wetted specific area of the packing and liquid side

345 Base Case T l

345
Base Case T v Base case T l
340 T exp 340 Base case T v
Case 1, T l Texp
335 335
Case 1, T v Case 6, T l
Case 2, T l Case 6, T v
T [K]

330
T [K]

330
Case 2, T v Case 7, T l
325
Case 3, T l 325
Case 7, T v
320 Case 3, T v Case 8, T l
320
Case 4, T l Case 8, T v
315 Case 4, T v 315
Case 9, T l
Case 5, T l
0 1 2 3 4 5 6 0 1 2 3 4 5 6 Case 9, T v
H, packing [m] Case 5, T v H, packing [m]

Fig. 3. Liquid and vapour phase temperature profiles inside the absorption tower Fig. 4. Liquid and vapour phase temperature profiles inside the absorption tower
for the Pilot Plant run 32, comparison of the predictions by the simulations case 1–5 for the Pilot Plant run 32, comparison of the predictions by the simulations cases
with the base case and experimental data. 6–9 with the base case and experimental data.
184 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189

360 absorption in the MEA solution is the better representation of the

CO2 consumption in the aqueous solution. The specific heat capac-
350 Base case, T l ity of the MEA solution decreases as ␣ increases. The temperature
T exp bulge predicted for pilot plant run 32 decreases compared to the
340
Case 4, T l
T l [K]

330
320
310
0 2 4 6
H, packing [m]
Fig. 5. Liquid phase temperature profiles inside the absorption tower for the Pilot
Plant run 47, comparison of the predictions by the simulation cases 4, 6 and 9 with
the base case and experimental data.
local mass transfer coefficient, and increases the liquid hold up and
enhancement factor. Slightly lower or unchanged values for  and
˛rich compared to the base case are observed for the pilot plant
cases with excess solution. Reduced transfer rates of H2 O and MEA
may have caused the larger temperature bulge compared to the
base case (Figs. 4 and 5).
In Case 7, when both the CO2 and H2 O transfer are considered,
the prediction of the temperature curves are not considerably dif-
ferent from the base case, and  and ˛rich are also very similar to
those from the base case. The possible explanation for this obser-
vation is the low volatility of MEA, which gives very little transfer
of MEA when it is considered. Therefore, absence of MEA transfer
has little effect on the model predictions.
Model predictions are almost identical to the base case pre-
dictions when all five species (CO2 , H2 O, MEA, N2 and O2 ) are
considered to be transferred between the phases (Case 8). Limited
solubility of N2 and O2 in the MEA solution should be the reason for
having almost negligible effects on the model predictions by the N2
and O2 phase transfer.
Inclusion of the minor reactions reported in literature (Kent
& Eisenberg, 1976) into the model (Case 9) has caused increased
 and ˛rich values. The possible explanation for increased CO2
base case, even though the reduced specific heat capacity should
Case 6, T l have resulted in an increased temperature bulge. Increased H2 O
Case 9, T l and MEA vaporization removes the heat that is generated by the
absorption of CO2 , which may have caused the smaller temperature
bulge for the pilot plant run 32.
The simulated results for ˛rich and  from various case simu-
lations are compared with the experimental values using parity
plots. The parity plots for ˛rich and  of all the cases are given in
Figs. 6 and 7, respectively. The prediction of ␣rich and  is improved
in Case 9, as seen by the parity plots, while the combination used
in Case 9 shows a tendency to under predict the temperature bulge
for the pilot plant cases with excess amine solution compared to
the CO2 inlet flow.
The sensitivity analysis shows that there is a considerable effect
from the selected correlations, reactions, and specie transfer on the
model predictions. The combination of the correlations used in the
base case simulations appear to have acceptable accuracy for the
absorption tower simulations.
5. Dynamic analysis
The analysis of the predictions from the dynamic model is based
on three simulations. The first simulation represents a plant start-
up scenario for the absorption column. The second simulation
represents the operation of the absorption column under varying
load conditions of the up-stream power plant, and the third sim-
ulation represents the influence from the stripping column on the
operation of the absorption column.
5.1. Start-up simulation
Several assumptions (adopted by Kvamsdal et al., 2009) and
simplifications are introduced in order to succeed with the

Bace case & Case 8 Case 1 Case 2

0.5 0.5 0.5

0.4 0.4 0.4

0.3 0.3 0.3

α CO , rich : Simulated

0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6
Case 3 Case 4 Case 5

0.5 0.5 0.5

0.4 0.4 0.4

0.3 0.3 0.3

2

0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6
Case 6 Case 7 Case 9

0.5 0.5 0.5

0.4 0.4 0.4

0.3 0.3 0.3

0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6 0.3 0.4 0.5 0.6
αCO , rich : Measured
2

Fig. 6. Parity plot of the rich CO2 loading for the base case and the nine cases used in the sensitivity analysis.
 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189 185

Base case & Case 8 Case 1 Case 2

100 100 100

80 80 80

60 60 60

40 40 40
40 60 80 100 40 60 80 100 40 60 80 100
Case 3 Case 4 Case 5
ηCO : Simulated
100 100 100

80 80 80

60 60 60
2

40 40 40
40 60 80 100 40 60 80 100 40 60 80 100
Case 6 Case 7 Case 9
100 100 100

80 80 80

60 60 60

40 40 40
40 60 80 100 40 60 80 100 40 60 80 100
ηCO 2 : Measured

Fig. 7. Parity plot of the percentage CO2 removal efficiency for the base case and the nine cases used in the sensitivity analysis.

simulation of the absorber for the plant start-up process. The main Gas and liquid velocities are set to extremely small values in
assumptions are given below: order to represent the no-flow conditions. The simulation proce-
dure of the start-up scenario is as follows:

• The column is filled with ambient air at the beginning.

• The liquid flow to the absorber (lean MEA) has a constant CO2 • The column filled with ambient air is simulated for 10 min.
loading. • Liquid flow starts at 10 min and reach the required value after
• The lean MEA flow is in reaction equilibrium. operating for 10 min (at 20 min).

t=0 t=0
(a) t = 20 min (b) t = 30 min
350 t = 30 min 0.5 t = 36 min
t = 43 min t = 43 min
340 t = 50 min t = 50 min
0.45
α CO [nCO / n MEA]

t = 120 min t = 120 min

330
0.4
T lAb [K]

320
0.35
2

310
0.3
300

290 0.25
0 2 4 6 0 2 4 6
H, packing [m] H, packing [m]

(c) (d)
0.5
α CO , rich [nCO / n MEA]

100
0.45
80
η CO [%]
2

0.4
60
2

0.35
40
2

0.3 20

0.25 0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
t [min] t [min]

Fig. 8. (a) Development of the liquid phase temperature profile inside the absorber during the start-up scenario, (b) change in the CO2 loading in the MEA solution inside the
absorber during the start-up scenario, (c) change in the CO2 loading in the rich MEA solution during the start-up scenario, (d) Change in the CO2 removal efficiency during
the start-up scenario.
186 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189

340 At first, the column filled with ambient air stays at the ambient
temperature. After the liquid flow is started, the column fills-up
with MEA at lean MEA temperature. When the gas flow is started,
330 the liquid phase is heated up as a result of the interfacial heat
transfer. A temperature bulge is developed as the CO2 absorption
is progressed due to the heat of absorption of CO2 into the solvent.
Change of the temperature value during the start-up scenario
320
with time at several positions of the column is given in Fig. 9. The
[K]

profiles show a smooth variation in the temperature with time.

Ab
Tl

Fig. 8c presents the change in rich loading (CO2 loading of the

310
300
290
0 20 40 60 80
t [min]
Fig. 9. Change of the liquid phase temperature with time at different positions of
the column, for the start-up scenario.
• Gas flow starts 5 min after the liquid flow becomes stable and
gains the required value after 25 min (at 50 min).
• The final flow rates are the same as the values used to simulate
the Pilot Plant run 32 from the Separations Research Program at
the University of Texas at Austin.
• The simulation covers 2 h of plant operation.
One of the main interests of such a simulation is the develop-
ment of the temperature profile of the tower during the start-up
process. Fig. 8a shows the development of the liquid phase tem-
perature profile whereas Fig. 8b shows the development of the CO2
loading profile during the start-up of the absorber along the height
of the column at some selected points in the time domain.
at 0.124 m solvent stream leaving the column) with time. The value of the rich
at 2.116 m loading increases as the gas flow into the column increases. The
at 4.108 m increase of the availability of CO2 to be absorbed is the reason for
the mentioned observation.
at 5.104 m
at 6.100 m The CO2 removal efficiency is an important quantity that draws
much attention with respect to the operation of a capture plant.
The change in the removal efficiency during the start-up process is
100 120 thus an interesting factor to point out. Fig. 8d shows the change in
CO2 removal efficiency during the start-up process.
Complete removal (100% efficiency) is noticeable just after the
introduction of the gas stream and shows a slow reduction until
a new steady state is reached with time. An explanation of the
observation is that almost all the CO2 could be absorbed at smaller
gas rates, and as the gas rate increases, the percentage removal
decreases depending on the absorption rate, contact time and phase
equilibrium.
Comparison of the steady state results of the simulation (once
the operation has become stable) with the pilot plant data gives
the results in Fig. 2b, thus confirming the reproducibility of the
predictions of the improved model.
5.2. Simulation of varying load conditions
The steady state results from the start-up scenario are used as
the initial conditions for this simulation. Firstly, the gas flow rate

t=0 t = 34 min
(a) t =15 min (b) t = 55 min
350 350
t = 22 min t = 58 min
t = 34 min t =120 min
340 340
T Ab [K]

T Ab [K]

330 330
l

320 320

310 310
0 2 4 6 0 2 4 6
H, packing [m] H, packing [m]
(c)
100

95
[%]

90
2
CO
η

85

80
0 50 100
t [min]

Fig. 10. (a) Development of the liquid phase temperature profile with the increased gas flow rate, (b) development of the liquid temperature profile with increased liquid
flow rate, (c) change in the CO2 removal efficiency during the varying load simulation.
 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189 187

350 changes, respectively, during the load varying situation. The tem-
at 0.124 m perature bulge appears to be increasing as the gas rate increases.
at 2.116 m This can be due to the increased amount of CO2 absorbed into a
340 at 4.108 m specific amount of MEA solution, which has increased the amount
at 5.104 m of heat released per specific amount of the solution. A change in the
T lAb [K]

at 6.100 m position of the temperature bulge is observed and the change is in

330
320
310
0 20 40 60 80
t [min]
Fig. 11. Change of the liquid phase temperature with time at different positions of
the column, for the varying load simulation.
into the absorption tower can be changed to introduce a vary-
ing load condition. Applying a varying gas flow rate is a suitable
approach for this type of simulation since this represents the pos-
sible variations in the up-stream power plant. Secondly, the liquid
flow can be changed in order to achieve the required removal effi-
ciency as this represents the possibility to regain the stability and
the controllability of the process.
The simulation procedure is given below:
• The base case is simulated for 10 min.
• The molar flow rate of gas is increased from 3.52 mol/s to
4.12 mol/s (≈17%) in 20 min (until t = 30 min).
• After 20 min, the liquid flow rate is changed from 40.73 mol/s to
60.73 mol/s (≈50%) over 20 min (until t = 1 h 10 min).
• The simulation keeps on for another 50 min (until t = 2 h).
The flow rates are changed linearly for the simulation rather
than introducing a step change, which represents a more sudden
change and more challenging operation.
Fig. 10a and b shows the change of the liquid phase temperature
profiles in the column as the gas rate changes and the liquid rate
accordance with the description of Kvamsdal and Rochelle (2008).
A reduction in the temperature bulge is observed as the liquid rate
increases. This can be explained as a result of the reduction of the
amount of specific heat release due to the CO2 absorption, even
though the absorption rate is increased.
100 120 Change of the temperature during the simulation at several
positions of the column is shown in Fig. 11. Profiles in Fig. 11
demonstrate smooth transient conditions for the temperature val-
ues due to the changes applied for the disturbance (gas rate) and
the input (liquid rate) at each of the points analyzed.
When the upstream power plant operates with varying loads,
the exhaust gas rate also varies. If the gas rate to the absorber
increases, the removal efficiency faces a drop due to the decreased
contact time. As a stabilizing effort, the liquid flow rate can be
increased accordingly to increase the absorption capacity while
forcing the efficiency to be back in the required operating range.
Fig. 10c shows the change in the removal efficiency with time dur-
ing the load varying operation of the capture plant.
5.3. Influence from the stripper
The steady state results from the start-up scenario are used
as the initial conditions for this simulation. A step change is
introduced to the lean CO2 loading value as an attempt to intro-
duce the influence from the down-stream stripping column. The
CO2 loading in the regenerated amine stream (the lean CO2 load-
ing) can vary due to possible variations in the stripping column
operation.
A step change is introduced for this simulation, which repre-
sents a more sudden change and more challenging operation, as a
measure of the capability of the model to handle such a situation.
The simulation procedure is given below:

(a) (b)
α CO , rich [nCO /nMEA]

100 0.45

0.44
2
η CO [%]

98
0.43
2

96
0.42
2

94 0.41
0 50 100 0 50 100
t [min] t [min]
(c)
350
at start
340 at 21.74 min
T lAb (K)

at 23.12 min
330
at 24.88 min
320

310
0 2 4 6
H, packing [m]

Fig. 12. (a) Change in the CO2 removal efficiency during the operation, (b) change in the rich CO2 loading during the operation, (c) development of the liquid phase temperature
profile with the decreased loading in the lean MEA stream.
188 S.A. Jayarathna et al. / Computers and Chemical Engineering 53 (2013) 178–189
345
at 0.124 m
340
at 0.996 m
at 1.949 m
335
at 2.241 m
at 3.112 m
330 at 4.357 m
Ab
at 5.602 m
Tl
325 at 6.100 m
320
315
310
0 10 20 30 40 50
t [min]
Fig. 13. Change of the liquid phase temperature with time at different positions of
the column, for the varying load simulation with a step change.
• The base case is simulated for 20 min.
• The CO2 loading in the lean MEA stream is changed from 0.28 to
0.24 mol CO2 /mol MEA.
Fig. 12a and b shows the change in the CO2 removal efficiency
and the rich CO2 loading with time due to the change in the lean CO2
loading, respectively. The removal efficiency shows a step increase
as the lean loading is dropped in a step. This must be a result of
the increased absorption capacity due to the reduced initial CO2
content in the solvent stream. A step decrease in the rich loading
is also observed. An obvious reason for the reduction of the rich
loading is the reduced initial CO2 content in the solvent stream
entering the column.
Fig. 12c shows the development of the liquid phase tempera-
ture profile inside the tower during the operation, and change of
the temperature with time at different positions of the column is
given in Fig. 13. Liquid temperature in the bottom half of the col-
umn shows a sudden increase (an over shoot) just after the step
change before settling down to a lower temperature value. The
developed temperature profiles after the step change have smaller
temperature bulges compared to the profile before the change. The
reason for the lower temperature value is the increased specific
heat capacity of the solution as a result of the reduced CO2 load-
ing. The over shoot in the temperature corresponding to the step
decrease in the lean loading demonstrates a challenging condition
(inverse response) if the temperature inside the column is to be
controlled within a specified range.
6. Conclusions
A good dynamic model provides the possibility to study the
effect of various disturbances on the operation of a plant and
to introduce improvements. Further, a dynamic model is useful
for implementing a control system for the plant and to perform
optimization, and for state estimation. Development of dynamic
models is vital for the understanding and improvement of the CO2
capture process.
The developed models must be solvable in fractions of real-
time, in order to be useful in an advanced control application (e.g.
MPC). Therefore, a balance between the computation burden and
the prediction accuracy is required.
A dynamic simulation model for the absorber of a CO2 cap-
ture plant is developed in order to predict the transient conditions
during various operating scenarios. The simplicity and low compu-
tation cost of the model is ensured by use of simple thermodynamic
models such as the Kent–Eisenberg model. The K–E model has been
published in detail with all necessary parameters elsewhere.
As primary validation step, model predictions are compared
with steady state data from the literature. The model predictions of
the steady state results are good even in absence of complex repre-
sentation of the thermodynamics. Further work is required related
to dynamic validation of the model. This will be performed by com-
paring it with the behaviour of a real plant; this is not included in
the current work due to the limitation in available data.
The results from the sensitivity analysis of the model shows
that there is a significant effect on the model predictions from the
combination of the correlations and reactions used, and the way of
representation of the inter-phase mass transfer in the model. The
combination of correlations used in the base case simulations is
selected for use in the absorption tower simulations.
60
Simulations are performed to analyze the start-up scenario,
plant operation under varying load and the influence from the strip-
ping column. The model predictions of the transient conditions
seem reasonable. The steady state results from the simulation of
the start-up scenario have shown good accordance with the pilot
plant data from the Separations Research Program at the University
of Texas at Austin.
The ultimate aim is to use our model for developing an on-line
control system for an amine based post-combustion CO2 capture
plant. The model will be expanded to cover the whole CO2 capture
plant; the expanded model will then be used for developing such a
control system for the capture process.
Acknowledgement
Financial support for this project from the Norwegian Research
Council is gratefully acknowledged.
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