chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228

Contents lists available at ScienceDirect

Chemical Engineering Research and Design

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

Pilot plant study of post-combustion carbon dioxide capture

by reactive absorption: Methodology, comparison of
different structured packings, and comprehensive results for
monoethanolamine

Hari Prasad Mangalapally, Hans Hasse ∗

Laboratory of Engineering Thermodynamics (LTD), University of Kaiserslautern, Kaiserslautern, Germany

a b s t r a c t

Post-combustion carbon capture (PCC) from fossil fuel power plants by reactive absorption can substantially con-
tribute to reduce emissions of the greenhouse gas CO2 . To test new solvents for this purpose small pilot plants
are used. The present paper describes results of comprehensive studies of the standard PCC solvent MEA (0.3 g/g
monoethanolamine in water) in a pilot plant in which the closed cycle of absorption/desorption process is continu-
ously operated (column diameters: 0.125 m, absorber/desorber packing height: 4.25/2.55 m, packing type: Sulzer BX
500, flue gas flow: 30–110 kg/h, CO2 partial pressure: 35–135 mbar). The data establish a base line for comparisons
with new solvents tested in the pilot plant and can be used for a validation of models of the PCC process with MEA.
The ratio of the solvent to the flue gas mass flow is systematically varied at constant CO2 removal rate, and CO2 par-
tial pressure in the flue gas. Optimal operating points are determined. In the present study the structured packing
Sulzer BX 500 is used. The experiments with the removal rate variation are carried out so that the results can directly
be compared to those from a previous study in the same plant that was carried out using Sulzer Mellapak 250.Y. A
strategy for identifying the influence of absorption kinetics on the results is proposed, which is based on a variation
of the gas load at a constant L/G ratio and provides valuable insight on the transferability of pilot plant results.
© 2011 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keywords: Amine; Carbon dioxide capture; Desorption; Flue gas; Mass transfer; Reactive absorption

1. Introduction
CO2 is a greenhouse gas and its emissions substantially
contribute to global warming. Therefore, the interest in tech-
niques which allow reducing CO2 emissions has tremendously
risen over the past years. According to the International
Energy Agency approximately one third of all CO2 emissions
come from the combustion of fossil fuels to generate electric-
ity (IEA, 2008). Employing carbon capture and storage (CCS) on
flue gases, especially from power plants, is one of the most
promising ways for mitigating the climate change. Among
the different CCS techniques, post-combustion carbon cap-
ture (PCC) is especially attractive for different reasons, the
most important of which is the possibility to retrofit exist-
ing power plants and the fact that there are existing technical
solutions and operational experience (CESAR, 2011). Compara-
tive assessments (IEA-GHG, 2000) have shown that absorption
based on chemical solvents is currently the preferred option
for PCC. The most widely used solvent for the process is
MEA (0.3 g/g monoethanolamine in water). The main disad-
vantage of MEA is high regeneration energy requirement,
which results in the high efficiency loss of the power plant.
Before PCC by reactive absorption can be employed on a
large scale and contribute to lowering of CO2 emissions from
power plants, better solvents will have to be found. This is
the aim of a large number of research projects carried out
world-wide (CASTOR, 2008; CESAR, 2011; BIGCO2, 2011; CCP,
2013; CO2CRC, 2015). In most of these studies MEA is chosen

∗
Corresponding author at: Laboratory of Engineering Thermodynamics (LTD), University of Kaiserslautern, Erwin-Schroedinger Strasse
44, P.O. Box 3049, 67663 Kaiserslautern, Germany. Tel.: +49 631 205 3497; fax: +49 631 205 3835.
E-mail addresses: hans.hasse@mv.uni-kl.de, mhariprasad23@gmail.com (H. Hasse).
Received 4 November 2010; Received in revised form 2 January 2011; Accepted 14 January 2011
0263-8762/$ – see front matter © 2011 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.cherd.2011.01.013
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228 1217

Table 1 – Main specifications of pilot plant.

Nomenclature
Parameter Data
Latin letters
Flue gas source Natural gas
HPacking height of packing burner
L/G ratio of solvent mass flow to flue gas mass flow CO2 content in the flue gas (vol%) (dry 3–14
captured
ṁCO captured CO2 mass flow rate basis)
2
ṁGL CO2 mass flow transferred from gas to liquid Flue gas flow rate (kg/h) 30–100
CO2
F-factor in absorber (Pa0.5 ) 0.6–2.1
ṁGL
H2 O H2 O mass flow transferred from gas to liquid
Solvent flow rate (kg/h) 20–350
ṁi mass flow of component i Liquid load in absorber (m3 /(m2 h)) 2–28.5
pi partial pressure of component i Inner diameter of pre-washer, absorber, 0.125
qReg regeneration energy per mass of captured CO2 desorber and washing sections (m)
T temperature Type of packing in the absorber and BX 500
(m) desorber
Xi mass fraction of component i
Total height of packing in the absorber (m) 4.25
XCO2 CO2 loading, in moles of CO2 per kg of unloaded
Total height of packing in the desorber (m) 2.55
solvent
Type of packing in the prewasher and Mellapak
absorber, desorber washing sections 250.Y
Greek letters Total height of packing in the pre-washer 0.84
CO2 CO2 removal rate (m)
Total height of packing in the washing 0.42
Superscripts sections of the absorber or desorber (m)
Abs absorber
abs absorbed available in Notz (2010) and are used here for a direct com-
Des desorber parison.
des desorbed Pilot plant studies with the solvent MEA have previously
G gas been described by Chapel et al. (1999), Knudsen et al. (2009),
GL gas to liquid Mangalapally et al. (2009), Mimura et al. (1995) and Tobiesen
in inlet et al. (2007, 2008). But, none of these covers the results in
L liquid comparable details as the present study.
m mass ratio
out outlet 2. Pilot plant and process description
Packing packing in the column
Reg regeneration
The process flow scheme of the absorption/desorption process
and the picture of the gas-fired pilot plant for post-combustion
Subscripts
CO2 capture by reactive absorption is shown in Fig. 1. The
CO2 carbon dioxide
main specifications of pilot plant are given in Table 1. The
i component i
flue gas produced by a gas burner is fed into the pre-washer
Solvent Amine + H2 O
column by a blower. The flue gas flow rate can be set approx-
imately between 30 kg/h and 150 kg/h. The maximum gas
flow rate through the absorber is limited to approximately
as a reference PCC solvent to which new solvents are com- 100 kg/h (F-factor (product of gas velocity and square root of
pared. gas density) ≈ 2.1 Pa0.5 ) due to fluid dynamic limitations. The
To test new solvents a gas-fired pilot plant is operated at pre-washer is built as a direct contact cooler to set the temper-
University of Kaiserslautern, Germany. The details of the pilot ature of the flue gas at the absorber inlet and at the same time
plant are described by Notz et al. (submitted for publication). to make sure that the flue gas is saturated with water. The
To obtain a baseline for testing new solvents, systematic stud- flue gas enters the absorber at the bottom with a temperature
ies are carried out with MEA in that plant in the present of approximately 40–50 ◦ C. The absorber is built of five sec-
work. In a first set of experiments the solvent flow rate is tions, which are each equipped with 0.85 m of the structured
varied at constant flue gas flow rate. Hence, the ratio of packing BX 500 (Sulzer Chemtec, Winterthur, Switzerland).
the two mass flow rates, the L/G ratio, is varied. In those The total packing height is 4.25 m. The regenerated solvent
experiments, the CO2 removal rate and CO2 partial pressure (lean solvent) is fed to the absorber top, typically at a temper-
in the flue gas are kept constant. Two levels of CO2 partial ature of 40 ◦ C. Upon the CO2 absorption into the liquid phase,
pressure are studied. For identifying the influence of mass absorption enthalpy is released, which leads to a temperature
transfer kinetics on the results, a second set of experiments increase. To reduce solvent loss by flue gas, there is a wash-
are carried out in which the gas load of the absorber (F- ing section at the absorber top above the solvent inlet. A low
factor) is varied while keeping the L/G ratio, CO2 removal amount of fresh deionized water is added into the washing
rate and CO2 partial pressure in the flue gas constant. Again, water recycle stream to avoid a prohibitive accumulation of
two levels of CO2 partial pressure are studied. In a third set amine in the washing water.
of experiments the CO2 removal rate is varied while keep- For steady state operation the liquid level in the absorber
ing the solvent mass flow rate, flue gas mass flow rate and bottom is controlled by a pump. The rich solvent is pumped
CO2 partial pressure in the flue gas constant. Experiments in into the desorber through the rich lean heat exchanger, where
the present study are carried out with the structured pack- the CO2 rich solvent is heated to higher temperatures through
ing Sulzer BX 500. Results for MEA obtained in the same the lean solvent from the desorber bottom. The desorber is
plant at similar conditions with Sulzer Mellapak 250.Y are built of three sections, which are each equipped with five ele-
1218 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228

Fig. 1 – (a) Flow scheme of the absorption/desorption process and (b) picture of the gas fired pilot plant for post-combustion
CO2 capture.

ments of BX 500 similar to the absorber. The total packing experiment. Two series of experiments are carried out: Series
height in the desorber is 2.55 m. Both the absorber and the des- A with the CO2 partial pressure of 54 mbar in the flue gas, cor-
orber columns have a diameter of 0.125 m. The bottom of the responding to gas-fired power plants; Series B with the CO2
desorber contains electrical heating elements for partial evap- partial pressure of 102 mbar in the flue gas, corresponding to
oration of the solvent. For aqueous amine solutions, mainly coal-fired power plants (Rolker and Arlt, 2006). For both series
water is evaporated. The vapor at the top of the desorber con- of experiments removal rate is specified as 90% by adjust-
sists of water, CO2 and some traces of amine. To retain the ing the reboiler duty. The main operating conditions of the
amine, also at the desorber top a washing section is installed. experiments are summarized in Table 3.
The vapor at the desorber top is led into the condenser where The reboiler duty measured in the experiments must be
most of the water is removed so that almost pure CO2 is corrected for heat losses. These are determined here using the
obtained. A part of the condensate is used in the washing sec- method proposed by Notz (2010). The heat losses are 1.5 kW
tion of the desorber and another part if necessary is withdrawn for experiments in which no flashing occurs in the rich/lean
to fulfill the water balance of the absorption/desorption pro- heat exchanger and 1.3 kW otherwise. The flashing regularly
cess. For a more detailed description of the pilot plant and its occurred for the experiments at the high CO2 partial pressure
operation, see Notz et al. (submitted for publication). due to limitations of the outlet pressure of pump P2. For a
discussion of the flashing, see Oyenekan and Rochelle (2006).
3. Pilot plant parameter study All numbers reported here for the heat duty are already cor-
rected for these losses. The numbers for the heat losses are
Overview of process parameter variation studies that are dis- in good agreement with those reported by Notz (2010) for his
cussed in the present paper are given in Table 2. The most experiments with MEA but with a different packing.
important process parameters affecting the capture process
for example L/G ratio, fluid dynamic load of the absorber (F-
factor) and CO2 removal rate are varied. Table 3 – Operating conditions of the experiments with
solvent flow variation. The temperature at absorber inlet
is 47 ◦ C for the flue gas and 40 ◦ C for the solvent. The
3.1. Variation of the L/G ratio F-factor is always 1.6 Pa0.5 and the CO2 removal rate is
always 90%.
In this set of experiments the solvent flow rate is varied at con- Process Series A Series B
stant flue gas flow rate. Hence, the ratio of the two mass flow variables
rates, the L/G ratio, is varied. The CO2 removal rate (CO2 ), CO2
CO2 partial 54 102
partial pressure and all other variables are fixed, cf. Table 2.
pressure in flue
As a direct setting of the CO2 removal rate is not possible it
gas (mbar)
has to be adjusted by suitably choosing the reboiler duty in an Flue gas mass 76 80
iterative process during each experiment. The reboiler duty at flow (kg/h)
the desired removal rate is the most important result of the Solvent mass 50–200 125–275
flow (kg/h)
Ratio of solvent 0.66–2.64 1.56–3.5
Table 2 – Overview of process parameter variation mass flow to
studies that are discussed in present paper. flue gas mass
flow (L/G)
Varied parameter Range of Constant parameters
variation (kg/kg)
CO2 mass flow in 6.2 12
L/G (kg/kg) 0.66–3.5 CO2 , pCO2 , ṁFluegas flue gas (kg/h)
F-factor (Pa0.5 ) 0.88–1.85 CO2 , L/G, pCO2 CO2 mass flow 5.5 10.5
CO2 removal rate (%) 40–90 pCO2 , ṁSolvent , ṁFluegas captured (kg/h)
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228
The results from the experiments with variation of the sol-
vent flow rate allow plotting the regeneration energy versus
the L/G ratio. From these plots an optimum solvent flow rate
and the corresponding minimum regeneration energy for a
given removal rate and CO2 partial pressure in the flue gas can
be found. The results depend not only on the specified removal
rate and the CO2 partial pressure but also on the plant design.
For exploring that influence, a second set of experiments are
carried out in which the fluid dynamic load of the absorber
(F-factor) is varied at a fixed L/G ratio.
3.2. Variation of the fluid dynamic load of the absorber
In this set of experiments, both the flue gas flow rate (F-factor)
and the solvent flow rate are varied simultaneously in a way
so that the ratio of both flow rates (L/G ratio) is kept con-
stant. As also all other variables like the CO2 removal rate,
CO2 partial pressure and the temperatures are kept constant
(cf. Table 2), this allows studying the influence of mass trans-
fer effects. Namely, upon decreasing the flow rates, also the
amount of the CO2 which is transferred between the gas and
the solvent decreases, both in the absorber and in the desor-
ber. Hence, less driving force for the mass transfer is needed, if
the interfacial area remains constant. Therefore, mass trans-
fer limitations will become less important, if they are present,
and can be identified. Note, that the available interfacial area
is also affected by the decreased fluid dynamic load. But the
slight decrease of the interfacial area upon decreasing the fluid
dynamic load only partially compensates the effect described
above.
Two series of experiments with a variation of the fluid
dynamic load are carried out: Series C with a CO2 partial pres-
sure in the flue gas of 54 mbar, corresponding to gas fired
power plants; Series D with a CO2 partial pressure in the
flue gas of 102 mbar, corresponding to coal fired power plants
(Rolker and Arlt, 2006). For both series of experiments removal
rate is 90%. The main operating conditions of the experiments
are summarized in Table 4. All experiments are carried out in
the recommended fluid dynamic operating range of the pack-
ing. The results from these experiments are analyzed in plot
of the regeneration energy versus the F-factor.
Table 4 – Operating conditions of the experiments with
flue gas flow rate variation. The temperature at absorber
inlet is 47 ◦ C for the flue gas and 40 ◦ C for the solvent.
The CO2 removal rate is always 90%.
Process Series C Series D
variables
CO2 partial 54 102
pressure in flue
gas (mbar)
Flue gas mass 40–85 40–80
flow (kg/h)
F-factor (Pa0.5 ) 0.88–1.85 0.88–1.72
Solvent mass 53–112 100–200
flow (kg/h)
Ratio of solvent 1.3 2.5
mass flow to
flue gas mass
flow (L/G)
(kg/kg)
CO2 mass flow in 3.2–7.1 6.1–11.7
flue gas (kg/h)
CO2 mass flow 2.9–6.4 5.6–10.6
captured (kg/h)
1219
3.3. Variation of the CO2 removal rate
In this set of experiments, the CO2 removal rate is varied by
adjusting the reboiler duty while all other variables like flue
gas flow rate, solvent flow rate, CO2 partial pressure and the
temperatures are kept constant, cf. Table 2. For these experi-
ments the CO2 partial pressure in the flue gas is maintained at
102 mbar. The experiments are carried out so that the results
can be directly compared to those from a previous study of
Notz (2010) carried out with Mellapak 250.Y. Table 5 shows
operating conditions for both studies. Despite the fact that
the flue gas volume flow is equal for all experiments, mass
flow in the experiments carried out with Mellapak 250.Y is
slightly lower than for the experiments with BX 500. This is
due to a different composition of the supplied natural gas.
The results from these experiments are analyzed in plot of
the regeneration energy versus the CO2 removal rate. This plot
allows comparing the absorption capacity of different column
internals.
4. Results and discussion
In the present paper, the experimental data is presented and
discussed using graphical representations in figures. A full set
of the experimental data determined in the present study is
reported as supplementary material and also can be seen in
Mangalapally (in preparation).
4.1. Variation of the L/G ratio
Fig. 2a shows the regeneration energy as a function of the ratio
of the solvent and the flue gas mass flow (L/G ratio) for the
experiments carried out with two different CO2 partial pres-
sures in the flue gas: 54 mbar and 102 mbar and with a CO2
removal rate of 90% (Series A and B, cf. Table 3). The results
at the high CO2 partial pressure given in Fig. 2 indicate an
optimum L/G ratio of about 2.5 corresponding to regeneration
energy of about 4.1 GJ/tCO2 . With the reduction of CO2 par-
tial pressure about to its half (i.e. from 102 mbar to 54 mbar),
the CO2 mass transferred from flue gas to the solvent is also
reduced to about its half (i.e. from 10.5 kg/h to 5.5 kg/h). As
a result the optimum L/G ratio is also reduced to about its
half. The corresponding number for MEA at the low CO2 par-
tial pressure is about 1.2 with regeneration energy of about
3.8 GJ/tCO2 . The increase in the regeneration energy to the left
of the optimum L/G ratio is related to the high amount of strip-
Table 5 – Operating conditions of the experiments with
CO2 removal rate variation. The temperature at absorber
inlet is 47 ◦ C for the flue gas and 40 ◦ C for the solvent.
The solvent mass flow is always 200 kg/h.
Process Mellapak 250.Y BX 500
variables
CO2 partial 109 102
pressure in flue
gas (mbar)
CO2 removal rate 40–88 58–90
(%)
Flue gas mass 75 80
flow (kg/h)
CO2 mass flow in 12 12
flue gas (kg/h)
CO2 mass flow 4.8–10.6 6.7–10.6
captured (kg/h)
1220 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228

Fig. 2 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on (a) specific regeneration energy, and (b)
CO2 loading of rich and lean solvent for experiments with low (䊉) and high () CO2 partial pressure in the flue gas (Series A
and B, cf. Table 3). In the experiments solvent flow rate is varied at constant flue gas flow rate, hence L/G ratio is varied. The
F-factor (flue gas flow rate) is always 1.6 Pa0.5 . The splines are guides for the eye.

ping stream demand. The increase in the regeneration energy
to the right of the optimum L/G ratio is mainly due to energy
requirement to heat up the higher solvent flows (Mangalapally
et al., 2009). The following sections give detailed results.
4.1.1. Rich and lean loadings
Fig. 2b shows the comparison of CO2 rich and lean load-
ings for MEA as a function of L/G ratio for experiments with
low and high CO2 partial pressure in the flue gas (Series A
and B, cf. Table 3). With the decreasing L/G ratio, the dif-
ference between CO2 loadings of the rich and lean solvent
must increase to fulfill the mass balance. At low L/G ratios
(below the optimum) the lean loading shifts to low values.
Low lean loadings in the desorber correspond to a difficult
separation task which results in a steep increase of the regen-
eration energy requirement cf. Fig. 2a (Abu-Zahra et al., 2007;
Mangalapally et al., 2009). For both low and high CO2 par-
tial pressure experiments (Series A and B, cf. Table 3), an
increase in the CO2 rich loadings is observed as L/G ratio is
decreased.
4.1.2. Absorber operating lines
Fig. 3 shows the comparison of absorber operating lines to
equilibrium curves as a function of L/G ratio for low and high
CO2 partial pressure experiments (Series A and B, cf. Table 3).
The absorber operating lines are estimated as explained by
Notz (2010) and Notz et al. (submitted for publication). These
estimates are based on primary experimental data and the
component mass balances and the energy balance for each
packing segment starting at the absorber bottom. The oper-
ating lines can only be plotted for the absorber, as the
experimental data for the CO2 partial pressure in the gas phase
is available, at the inlet and outlet of the absorber, which is
not the case for the desorber. Together with the operating
lines also the equilibrium curves at 40 ◦ C, 50 ◦ C and 60 ◦ C are
shown (temperatures in the absorber sump vary from 45 ◦ C to
55 ◦ C). The CO2 loading is given in mol CO2 /kg solvent. This
unit is chosen, so that the influence of the solvent mass flow
pumped around in the absorption/desorption process can be
seen easily. The distance between the operating line and the
equilibrium curve gives an indication of the driving force for
the mass transfer. As expected, the slope of the operating line
decreases as L/G decreases. With decreasing L/G, the lower
end point of the operating line (corresponding to the absorber
top) always shifts to lower (lean) loadings, while the upper end
point of the operating line (corresponding to the absorber bot-
tom) shifts to higher (rich) loadings. This holds for both the
low and the high CO2 partial pressure experiments.
4.1.3. Energy contributions to the regeneration energy
Fig. 4 shows the influence of L/G ratio on four different con-
tributions to the regeneration energy, namely: the energy
needed for (1) desorption of CO2 (desorption enthalpy), (2)
generating stripping stream, (3) heating up of the solvent,
and (4) heating up of the reflux condensate. The estimation
of these four contributions is based on the evaluation of the
different terms in the desorber energy balance as explained
in detail by Notz (2010). The specific desorption enthalpy
mainly depends on the temperature if the CO2 loading is
less than 0.5 molCO2 /molMEA (Kim and Svendsen, 2007) and
thus is expected to be almost constant for the experimental
conditions in this L/G ratio variation study. In addition the
reflux condensate flow at the top of the desorber is small,
so that the optimum L/G ratio depends mainly on the energy
requirement for the stripping stream and for heating up the
solvent.
Results shown in Fig. 4a and b show similar behaviour for
both low and high CO2 partial pressure experiments (Series
A and B, cf. Table 3). Details are discussed considering only
the results from high CO2 partial pressure experiments (Series
B, cf. Table 3). As expected, the energy required for desorp-
tion of CO2 (desorption enthalpy) remains almost constant
upon increasing the L/G ratio. The increase in the energy
requirement for the stripping stream at low L/G ratios is due
to the high stripping stream demand. The slight increase
in the stripping stream demand at high L/G ratios is due
to the fact that the water vapor stream at the outlet of
the desorber washing section is interpreted as the stripping
stream. The water vapor stream is estimated based on the
vapor pressure curve of water using the temperature at the
outlet of desorber washing section. Therefore, the energy
contribution to the stripping stream is determined by the
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228 1221

Fig. 3 – Comparison of absorber operating lines to equilibrium curves at 40 ◦ C, 50 ◦ C and 60 ◦ C for L/G ratio variation
experiments with (a) low CO2 partial pressure in the flue gas (Series A, cf. Table 3), L/G: 1.0 (♦), 2.0 () and 2.6 (), and (b)
high CO2 partial pressure in the flue gas (Series B, cf. Table 3), L/G: 1.9 (♦), 2.5 () and 3.5 (). The F-factor (flue gas flow rate)
is always 1.6 Pa0.5 . The splines are guides for the eye. Equilibrium data from Notz (2010).

temperature at the outlet of desorber washing section. Gen-
erally, with the increase of the L/G ratio the energy required
to heat up the solvent increases, as shown in Fig. 4a and
b.
Fig. 5 shows the four different energy contributions to the
total regeneration energy, for the optimum L/G ratios of low
and high CO2 partial pressure experiments (Series A and B,
cf. Fig. 2a). The main contribution is the energy needed to
supply the desorption enthalpy of CO2 . The resulting num-
bers are same for both series of experiments at optimum L/G
ratio (Series A: 2.29 GJ/tCO2 , Series B: 2.29 GJ/tCO2 ) which is
in line with the observation that the enthalpy of absorption
for an aqueous solution of 0.3 g/g MEA is almost indepen-
dent of the CO2 loading up to a value of approximately
0.5 molCO2 /molMEA (Kim and Svendsen, 2007). As the opti-
mum L/G ratio is doubled for the high CO2 partial pressure
experiments compared to low CO2 partial pressure experi-
ments, the energy required for heating up the solvent flow
rate is also doubled, the corresponding numbers are (Series
A: 0.21 GJ/tCO2 , Series B: 0.46 GJ/tCO2 ). The energy needed
to supply stripping stream and the energy needed to heat
up the reflux condensate are similar for both low and high
CO2 partial pressure experiments at optimum L/G ratios, as
shown in Fig. 5. It has to be kept in mind, that the abso-
lute numbers of the latter three contributions to the specific
energy requirement are plant specific. They may differ for
large scale plants depending on the design. Nevertheless, it
can be concluded that the enthalpy of absorption and the
stripping stream requirement are the main contributions to
the regeneration energy requirement followed by the energy
for heating up the solvent and reflux condensate in the des-
orber.

Fig. 4 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on four different contributions to the
regeneration energy, namely desorption of CO2 (), stripping stream (), heating of the solvent (♦) and heating of the reflux
condensate (). Data for L/G ratio variation experiments with (a) low CO2 partial pressure in the flue gas (Series A, cf.
Table 3), and (b) high CO2 partial pressure in the flue gas (Series B, cf. Table 3) in the flue gas. The F-factor (flue gas flow rate)
is always 1.6 Pa0.5 . The splines are guides for the eye.
1222 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228
Fig. 5 – Four different contributions to the regeneration energy for experiments with (a) low CO2 partial pressure in the flue
gas, at optimum L/G: 1.2 (Series A, cf. Table 3), and (b) high CO2 partial pressure in the flue gas at optimum L/G: 2.5 (Series B,
cf. Table 3). The F-factor (flue gas flow rate) is always 1.6 Pa0.5 .
4.1.4. Temperature and concentration profiles
Figs. 6 and 7 show absorber and desorber temperature and CO2
concentration profiles as a function of the L/G ratio for experi-
ments with high CO2 partial pressure in the flue gas (Series
B, cf. Table 3). Very similar results are obtained for experi-
ments with low CO2 partial pressure in the flue gas (Series
A, cf. Table 3) and are not discussed here in detail for brevity.
For plots, see Mangalapally (in preparation).
Fig. 6 gives the results for the absorber. For high L/G ratios
most of the CO2 absorption takes place in lower part of the
absorber column resulting in a larger temperature bulge. As a
result high liquid temperatures are observed in the absorber
bottom for high L/G ratios, cf. Fig. 6a. For low L/G ratios, the
temperature bulge is smaller and the temperature maximum
is nearer to the top of the column, since more CO2 absorption
takes place in the upper part of the absorber column. As a
result, higher gas temperatures are observed in the absorber
top for low L/G ratios, cf. Fig. 6a (filled symbols).
Fig. 6b shows the liquid phase mass fraction profiles of CO2
measured in the absorber as a function of the L/G ratio. The
results for the mass fraction profiles of CO2 in the absorber are
in line with the temperature profiles. As mentioned above, at
high L/G ratios most of the CO2 absorption takes place in the
lower part of the absorber (see the concentration gradient in
Fig. 6b), resulting in higher temperature in the absorber bot-
tom. High temperatures correspond to lower CO2 loadings. At
low L/G ratios more CO2 absorption takes place in the upper
part of the absorber (see the concentration gradient in Fig. 6b).
As a result lower temperatures are observed in the absorber
bottom, corresponding to higher CO2 loadings.
Fig. 7 gives the results for the desorber. The desorber tem-
perature profiles as a function of L/G ratio are shown in Fig. 7a,
and the liquid phase CO2 mass fraction profiles as a function
of L/G ratio are shown in Fig. 7b. At high L/G ratio (L/G = 3.5)
temperature typically decreases rapidly between the bottom
and the middle section of the desorber, which indicates that
most of the CO2 is released in the lower section, cf. Fig. 7a.
Between the middle and top section only a minor tempera-
ture change is seen. At L/G = 2.5, the temperature decrease is
almost linear through out the desorber column, which indi-
cates an optimal use of the desorber. At L/G ratio 1.9, the
temperature decreases rapidly between the middle and the
top section, which indicates that most of the CO2 is released
in the upper section of the desorber. Between the bottom and
middle section only a minor temperature change is observed.
Similarly to the absorber, also for the desorber the tempera-
ture and the CO2 mass fraction profiles are directly coupled.
The CO2 mass fraction profiles measured in the desorber at
different L/G ratios are in line with the temperature profiles.
4.1.5. Partial pressure profiles in the absorber
From the primary experimental data estimates can be
obtained for the H2 O and CO2 partial pressure profiles in the
columns as explained by Notz (2010) and Notz et al. (submitted
for publication). Results for the absorber are plotted in Fig. 8
as a function of the L/G ratio for experiments with high CO2
partial pressure in the flue gas (Series B, cf. Table 3). The par-
tial pressure profiles of the experiments with low CO2 partial
pressure in the flue gas (Series A, cf. Table 3), which are not
reported here, show similar behaviour. The partial pressure
profiles of water as a function of L/G ratio show close relation
to the temperature profiles (compare Figs. 6 and 8a). Whereas
the partial pressure profiles of CO2 as a function of L/G ratio
show close relation to the CO2 mass fraction profiles (compare
Figs. 6 and 8b).
4.1.6. Mass transfer profiles in the absorber
From the primary experimental data estimates can be
obtained for the H2 O and CO2 mass transfer profiles in the
absorber as explained by Notz (2010) and Notz et al. (submitted
for publication). The estimate is based on the measurement
of the profiles for the temperature and the CO2 mass fraction
in the liquid phase. Additionally, the flow rate and the com-
position of gas and liquid stream at the bottom are required
as input. It is assumed that only CO2 and H2 O show a sig-
nificant mass transfer. The component mass balance and the
energy balance are solved for each packing segment starting
at the bottom. In the washing section, only H2 O mass transfer
is considered.
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228 1223

Fig. 6 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on absorber profiles for experiments with
high CO2 partial pressure in the flue gas (Series B, cf. Table 3): (a) liquid phase temperature profiles and gas phase
temperature profiles (filled symbols), and (b) liquid phase CO2 mass fraction profiles. Data for L/G: 1.9 (♦), 2.5 () and 3.5 ().
The F-factor (flue gas flow rate) is always 1.6 Pa0.5 . The splines are guides for the eye.

Results for the absorber are plotted in Fig. 9 as a function
of L/G ratio for experiments with high CO2 partial pressure in
the flue gas (Series B, cf. Table 3). The mass transfer profiles for
the experiments with low CO2 partial pressure in the flue gas
(Series A, cf. Table 3) which are not reported here show similar
behaviour.
The mass transfer profiles of water from gas to liquid as
presented in Fig. 9a show that in the lower part of the absorber
the gas stream takes up water, whereas in the upper part of the
absorber water vapor from the gas stream condensates. This
behaviour is related to the temperature profile in the absorber;
cf. Fig. 6a, which determines the equilibrium partial pressure
of water in the gas phase. For high L/G ratios a high mass flow
of water is taken by the gas stream in the lower part of the
absorber and a high mass flow of water vapor is condensed
from the gas stream in the upper part of the absorber. Simi-
larly, for low L/G ratios a low mass flow of water is taken by the
gas stream in the lower part of the absorber and a low mass
flow of water vapor is condensed from the gas stream in the
upper part of the absorber.
Fig. 9b shows the mass transfer profiles of CO2 from gas
to liquid in the absorber as a function of the L/G ratio. As
expected, if the L/G ratio is varied, a shift of the importance
of different parts of the column for the CO2 mass transfer is
observed. Upon decreasing the L/G ratio, the upper part of the
absorber becomes relatively more important.
4.2. Variation of the fluid dynamic load of the absorber
Up to now, only results from series of experiments in which
the flue gas flow rate is constant are discussed. In those exper-
iments the flue gas flow rate is chosen so that the packing have

Fig. 7 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on desorber profiles for experiments with
high CO2 partial pressure in the flue gas (Series B, cf. Table 3): (a) liquid phase temperature profiles and gas phase
temperature profiles (filled symbols), and (b) liquid phase CO2 mass fraction profiles. Data for L/G: 1.9 (♦), 2.5 () and 3.5 ().
The F-factor (flue gas flow rate) is always 1.6 Pa0.5 . The splines are guides for the eye.
1224 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228

Fig. 8 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on absorber profiles for experiments with
high CO2 partial pressure in the flue gas (Series B, cf. Table 3): (a) H2 O partial pressures, and (b) CO2 partial pressures. Data
for L/G: 1.9 (♦), 2.5 () and 3.5 (). The F-factor (flue gas flow rate) is always 1.6 Pa0.5 . The splines are guides for the eye.

a reasonably high fluid dynamic load, the F-factor is always
1.6 Pa0.5 .
In the set of experiments which are discussed in the
present section both the flue gas flow rate (F-factor) and
the solvent flow rate are varied, but the ratio of the flow
rates, i.e. the L/G ratio is kept constant. As also all other
parameters like the CO2 removal rate, CO2 partial pressure
in the flue gas and feed temperatures are kept constant (cf.
Table 2), this allows studying kinetic effects. Upon reduc-
ing the flue gas flow rate at constant removal rate, the
CO2 mass flow in the flue gas is reduced and so is the
CO2 mass flow which has to be transferred between the
gas and the liquid phase, both in the absorber and in the
desorber. As a consequence, a lower driving force is suffi-
cient at lower flue gas flow rates and it is expected that
the absorber operating line is shifted to higher loadings,
which results in a reduction of stripping stream demand
and thus in a reduction of total regeneration energy. It
should be noted that with decreasing flue gas and sol-
vent flow rates the effective interfacial area decreases
(Hoffmann et al., 2007; Tsai et al., 2009; Weimer and Schaber,
1996). This only partially compensates the effect described
above.
Fig. 10a shows the regeneration energy as a function of the
fluid dynamic load of the absorber (F-factor) for the experi-
ments carried out with two different CO2 partial pressures in
the flue gas: 54 mbar and 102 mbar at a CO2 removal rate of
90% (Series C and D, cf. Table 4). The L/G ratio is kept constant
at 1.3 for the experiments with low CO2 partial pressure in
the flue gas, which is the optimum found from the L/G ratio
variation studies (cf. Fig. 2a). For the same reason the L/G ratio
for the experiments with high CO2 partial pressure in the flue
gas is kept constant at 2.5. The results show the expected
decrease of the regeneration energy with decreasing F-factor.
The slope is similar for both sets of experiments. This con-
cludes that the change in CO2 partial pressure in the flue gas

Fig. 9 – Influence of the ratio of solvent mass flow to flue gas mass flow (L/G ratio) on absorber profiles for experiments with
high CO2 partial pressure in the flue gas (Series B, cf. Table 3): (a) mass transfer profiles of H2 O from gas to liquid, and (b)
mass transfer profiles of CO2 from gas to liquid. Data for L/G: 1.9 (♦), 2.5 () and 3.5 (). The F-factor (flue gas flow rate) is
always 1.6 Pa0.5 . The splines are guides for the eye.
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228 1225

Fig. 10 – Influence of the fluid dynamic gas load of the absorber (F-factor) on (a) specific regeneration energy, and (b) CO2
loading of rich and lean solvent for experiments with low (䊉) and high () CO2 partial pressure in flue gas (Series C and D,
cf. Table 4). In the experiments, the flue gas flow rate is varied but the L/G ratio is kept constant. The L/G ratio is 1.3 for
experiments with low (䊉) and 2.5 for the experiments with high () CO2 partial pressure in the flue gas. The splines are
guides for the eye.

does not have major influence on the overall mass transfer the interfacial area available in the absorber is ample for that
kinetics of the solvent. The following sections give detailed separation.
results.

4.2.2. Absorber operating lines

4.2.1. Rich and lean loadings
Fig. 10b shows the comparison of CO2 rich and lean loadings
for MEA as a function of F-factor for experiments with low
and high CO2 partial pressure in the flue gas (Series C and D,
cf. Table 4). With the decrease of F-factor, the CO2 rich and
lean loadings increase, but the difference between the CO2
loadings of the rich and the lean solvent is constant, since the
CO2 removal rate and the L/G ratio are kept constant. Note
that for experiments at low CO2 partial pressure in the flue
gas, the CO2 loadings remain almost constant upon decreasing
the F-factor, cf. Fig. 10b. This is a consequence of the fact that
Fig. 11 shows the shift of the absorber operating lines towards
equilibrium curves upon decreasing the F-factor as measured
for experiments with low and high CO2 partial pressure in
the flue gas (Series C and D, cf. Table 4). Together with the
operating lines also the equilibrium curves at 40 ◦ C, 50 ◦ C and
60 ◦ C are shown (the temperatures in the absorber sump vary
from 45 ◦ C to 55 ◦ C). The expected shift towards the absorber
equilibrium curves is observed for experiments with high CO2
partial pressure in the flue gas. But, for experiments with low
CO2 partial pressure in the flue gas the absorber operating
lines do not show much shift upon decreasing the F-factor.

Fig. 11 – Comparison of absorber operating lines to equilibrium curves at 40 ◦ C, 50 ◦ C and 60 ◦ C for the flue gas flow
variation experiments with (a) low CO2 partial pressure in the flue gas (Series C, cf. Table 4), F-factor: 1.33 (♦), 1.64 () and
1.85 (), and (b) high CO2 partial pressure in the flue gas (Series D, cf. Table 4), F-factor: 0.88 (♦), 1.28 () and 1.69 (). The
L/G ratio is 1.3 for experiments with low (䊉) and 2.5 for the experiments with high () CO2 partial pressure in the flue gas.
The splines are guides for the eye. Equilibrium data from Notz (2010).
1226 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228

Fig. 12 – Influence of CO2 removal rate on: (a) specific regeneration energy, and (b) CO2 loading of rich and lean solvent for
experiments with different column internals. Comparison of experimental results for BX 500 () from the present work
with experimental data for Mellapak 250.Y (䊉) from Notz (2010) taken at similar conditions. In the experiments, the CO2
removal rate is varied but the flue gas mass flow rate and solvent mass flow rate is kept constant (cf. Table 5). The splines
are guides for the eye.

As mentioned in Section 4.2.1, this is consequence of avail-
ability of ample packing height in the absorber column which
allows closely approaching the equilibrium CO2 loading.
4.3. Variation of the CO2 removal rate and comparison
of different column internals
Up to now, only results from series of experiments in which
the CO2 removal rate is constant are discussed. In the fol-
lowing, results from a series of experiments are presented, in
which the CO2 removal rate is varied at constant CO2 partial
pressure, flue gas flow rate, solvent mass flow rate, cf. Table 5.
The results from the current study with column internal
Sulzer BX 500 are compared with results from a similar series
of experiments that are carried out by Notz, 2010 in the
same pilot plant at similar conditions with column internal
Mellapak 250.Y, cf. Table 5.
Fig. 12a shows the comparison of results for the regenera-
tion energy for Mellapak 250.Y and BX 500. For both packings,
the regeneration energy demand is similar for removal rates
less than 76%. For these low removal rates the columns are
amply designed in both cases, equilibrium is almost reached,
and, hence, no differences can occur. For removal rates above
76%, the increase of the regeneration energy demand upon

Fig. 13 – Comparison of absorber operating lines to equilibrium curves at 40 ◦ C, 50 ◦ C and 60 ◦ C for the CO2 removal rate
variation experiments with different column internals: (a) results for Mellapak 250.Y from Notz (2010) taken at similar
conditions, CO2 : 40% (), 51% (), 76% () and 88% (♦), and (b) results for BX 500 from present study, CO2 : 58% (), 77% ()
and 90% (♦). The splines are guides for the eye. The calculated equilibrium curves with no symbols for MEA are from Notz
(2010).
 chemical engineering research and design 8 9 ( 2 0 1 1 ) 1216–1228
increasing the CO2 removal rate is drastic for the experiments
with Mellapak 250.Y, whereas, for BX 500, because of its much
higher surface area, low numbers of the regeneration energy
are found at higher removal rates. The following sections give
detailed results.
4.3.1. Rich and lean loadings
Fig. 12b shows the comparison of CO2 rich and lean loadings as
a function of CO2 removal rate for Mellapak 250.Y and BX 500.
Upon increasing the CO2 removal rate the loading difference
between rich and lean solvent increases for both Mellapak
250.Y and BX 500. For high removal rates there are differences
between Mellapak 250.Y and BX 500. For Mellapak 250.Y, lower
values of the rich loading are observed. This is due to the lack
of sufficient interfacial area for the mass transfer between the
flue gas and the solvent in the absorber, which causes that
the equilibrium is not reached. The loading difference is fixed
for a given solvent flow rate, flue gas flow rate, and removal
rate. Therefore, lean loadings are also shifted to low values for
Mellapak 250.Y. For attaining these low lean loadings in the
desorber, high regeneration energies are needed. Contrarily
to Mellapak 250.Y, sufficient interfacial area for mass trans-
fer is provided by the BX 500 packing so that the rich loading
remains almost constant even at high removal rates.
4.3.2. Absorber operating lines
Fig. 13 shows the comparison of absorber operating lines to
equilibrium curves as a function of CO2 removal rate for exper-
iments with column internals Mellapak 250.Y and BX 500 (cf.
Table 5). Together with the operating lines also the equilibrium
curves at 40 ◦ C, 50 ◦ C and 60 ◦ C are shown (temperatures in the
absorber sump vary from 45 ◦ C to 55 ◦ C). In the experiments
with Mellapak 250.Y, upon increasing the CO2 removal rate the
absorber operating line shifts to lower loadings, as a greater
driving force for mass transfer is required, cf. Fig. 13a. The shift
of the absorber operating line is drastic for removal rates above
76%, because of the lack of sufficient interfacial area for the
mass transfer which results in a drastic increase in the regen-
eration energy. Contrarily to Mellapak 250.Y sufficient interfa-
cial area for mass transfer is provided by the BX 500 packing
so that the rich loading remains almost constant even at high
removal rates. As a consequence, only the lean loadings shift
to lower numbers upon increasing the CO2 removal rate result-
ing in an ovelap of the absorber operating lines, cf. Fig. 13b.
5. Conclusions
The present paper reports on results of a systematic base line
study with MEA in a pilot plant. Three different sets of exper-
iments are carried out. In each set of experiments two series
are carried out at two different levels of CO2 partial pressure
in flue gas.
In first set of experiments, the solvent flow rate is varied at
constant flue gas flow rate. Hence, the ratio of the two mass
flow rates, L/G ratio, is varied; at constant partial pressure of
CO2 in the flue gas and constant CO2 removal rate. The opti-
mal L/G ratio leading to a minimum energy requirement is
determined through this set of experiments. The results from
this data set can be used as a base line for comparing with
results of new solvents. Note that the absolute numbers for
the optimal L/G ratio and regeneration energy depend not only
on the specified partial pressure of CO2 in the flue gas and the
CO2 removal rate but also on the design of the pilot plant. To
explore that influence, a second set of experiments is carried
1227
out in which the flue gas flow rate is varied at a constant ratio
of the solvent mass flow to the flue gas mass flow (L/G ratio)
and a constant removal rate and partial pressure of CO2 in the
flue gas. Low flue gas flow rates lead to a low mass flow of
captured CO2 , so that the amount of CO2 that has to be trans-
ferred per second through the interfacial area decreases. The
effect of lowering the flue gas flow rate in the way described
above is, hence, similar to that of increasing the column height
at constant flue gas flow rate. The results show an influence
of overall mass transfer kinetics even for MEA, which is often
said to be a fast solvent. They also show that the kinetic effects
do not strongly depend on the level of the CO2 partial pressure
in the flue gas.
In a third set of experiments, the CO2 removal rate is varied
at constant solvent mass flow, flue gas mass flow and CO2 par-
tial pressure in the flue gas. Data from the present study with
BX 500 are compared to those obtained using a less efficient
packing, Mellapak 250.Y. The results show that at low CO2
removal rates both packings yield almost the same results,
whereas at high removal rates, the advantages of BX 500 are
significant. For the pilot plant used in the present work, a CO2
removal rate of 90% cannot be reached with reasonable regen-
eration energy using Mellapak 250.Y whereas this poses no
problem with the BX 500 packing.
The procedures described here can also be applied to new
solvents and yielded data allow safe comparisons of solvents
based on pilot plant investigations.
Acknowledgment
This work is mainly carried out under the European Com-
mission’s 7th Framework Program Integrated Project CESAR
(FP7/2007-2011) under Grant Agreement No. 213569.
Appendix A. Supplementary data
Supplementary data associated with this article can be found,
in the online version, at doi:10.1016/j.cherd.2011.01.013.
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