International Journal of Greenhouse Gas Control 39 (2015) 194204

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International Journal of Greenhouse Gas Control

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

Investigating the inuence of the pressure distribution in a

membrane module on the cascaded membrane system for
post-combustion capture
Torsten Brinkmann a , Jan Pohlmann a , Martin Bram b , Li Zhao b, , Akos Tota c ,
Natividad Jordan Escalona d , Marijke de Graaff e , Detlef Stolten b,f
a
Institute of Polymer Research, Helmholtz-Zentrum Geesthacht, Max-Planck- Str. 1, D-21502 Geesthacht, Germany
b
Institute of Energy and Climate Research, Forschungszentrum Jlich, D-52425 Jlich, Germany
c
Linde Engineering, D-82049 Pullach, Germany
d
RWE Power Aktiengesellschaft, D-45128 Essen, Germany
e
EnBW Energie Baden-Wrttemberg AG, Durlacher Allee 93, D-76131 Karlsruhe, Germany
f
Chair for Fuel Cells, RWTH Aachen University, D-52056 Aachen, Germany

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

Article history: Polyactive membranes show promising properties for CO2 separation from ue gas. An investigation of
Received 24 July 2014 different module types using Polyactive membranes was carried out for this paper. A test rig was built
Accepted 12 March 2015 to explore, amongst other process parameters, the pressure drop in envelope-type membrane modules.
The experimental data and simulation results were compared with quite good consistency. This valida-
Keywords: tion enabled further simulations for different modules in a virtual pilot plant conguration. Applying the
Carbon capture
data from the pilot plant simulation to a reference power plant, the scaled-up cascaded membrane sys-
Gas separation
tem was analyzed using different membrane modules. Considering the required membrane area, energy
Membrane module
Pressure drop
consumption and pressure drop in different modules, a counter-current membrane module congura-
Efciency loss tion exhibited the best performance and had a marginal advantage in comparison with the chemical
Post-combustion absorption process.
2015 Elsevier Ltd. All rights reserved.

1. Introduction
Energy-related CO2 emissions reached a record 31.2 gigatonnes
in 2011, representing by far the largest source (around 60%) of
global greenhouse-gas emissions measured on a CO2 -equivalent
basis (World Energy Outlook, 2012). An update released by the
World Bank warns about the potentially disastrous consequences
that an increase of four degrees Celsius in the global temperature
could have by 2100 (World Could Be 4 Degrees Hotter By End of This
Century, 2013). Forecasts by the IEA and others show that decar-
bonizing electricity and enhancing end-use efciency could make
major contributions to the ght against climate change (Climate
Electricity Annual, 2011). In spite of increased energy efciency,
the electricity demand is projected to increase substantially by
up to 50% between today and 2050. Renewable energy systems
(RES) will generate at least 40% of the electricity required to meet
this demand, and the rest will be generated by nuclear sources and
Corresponding author. Tel.: +49 2461 614064; fax: +49 2461 616695.
E-mail address: l.zhao@fz-juelich.de (L. Zhao).
fossils with carbon capture and storage (CCS) (Decarbonizing the
European Electric Power Sector by 2050). CCS is a series of technolo-
gies and applications which capture CO2 from large point sources,
transport it via pipelines and ships and safely store it in geological
formations, such as saline aquifers and depleted oil and gas elds
(Metz et al., 2005a).
The principle of CCS is clear: continue using fossil fuels and
capture and store the released CO2 underground. However, the
technology is currently still being developed and has yet to be
demonstrated as feasible on a large scale at acceptable cost. Apart
from high investment costs, a high CO2 price or regulations will be
required to encourage actual use of CCS, as a signicant share of the
power generated by a CCS plant is needed to drive its gas separa-
tion units, thereby lowering the plants net efciency and exibility
(Decarbonizing the European Electric Power Sector by 2050). In
different regions in the world, post-combustion, pre-combustion
and oxy-fuel combustion processes are considered options for CO2
capture in the large-scale demonstration of CCS in the power gen-
eration sector. To date, no individual capture route or technology
can claim a general competitive advantage over other processes
(Climate Electricity Annual, 2011).

http://dx.doi.org/10.1016/j.ijggc.2015.03.010
1750-5836/ 2015 Elsevier Ltd. All rights reserved.
 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204
Fig. 1. Types of investigated membrane modules.
The competing technologies for post-combustion carbon cap-
ture are absorption, adsorption and membrane methods (Metz
et al., 2005a; Post-Combustion CO2 Control U.S. Department of
Energy, 2014). As the rst-generation technology for CO2 capture,
amine absorption is a mature and proven purication technique
that is widely employed in the industrial treatment of acid gases
(Kohl and Nielsen, 1997). Nevertheless, the high energy consump-
tion of the absorbent (monoethanolamine, MEA) regeneration step
with efciency losses of 1014% points and corrosion problems
associated with solvent degradation increase the operation and
maintenance costs of this technology (Wang et al., 2011; Luis et al.,
2012; Mangalapally et al., 2012; Svendsen et al., 2011; Blomen
et al., 2009; Galindo-Cifre et al., 2009). Gas separation membrane
technologies, a potential second-generation technology for post-
combustion capture, are gaining more and more attention. The
advantages of these technologies are their potentially lower envi-
ronmental impact and the fact that membrane modules can be
used as add-on equipment requiring with fewer modications
to power plants. The other potential advantage is that for low
degrees of CO2 separation, a membrane array demands a lower
specic energy than that required for MEA absorption. Further-
more, membrane systems are easier to scale-up and more suitable
for intermittent, dynamic operation. Membrane science and tech-
nology can be divided into two classes, namely materials research
and process engineering. Many groups and researchers world-
wide have been involved in materials and process development
(Zhao et al., 2010; Bounaceur et al., 2006; Favre, 2007; Car et al.,
2008a; Follmann et al., 2011; Ho et al., 2008; Deng et al., 2009;
Hussain and Hgg, 2010; Merkel et al., 2010; Brinkmann et al., 2011;
Kai et al., 2008; Powell and Qiao, 2006; Lin and Freeman, 2005;
Reijerkerk et al., 2010; Brunetti et al., 2010; Bram et al., 2011), with
some institutions covering the entire research and development
chain from material synthesis to process engineering (Hussain and
195
Hgg, 2010; Merkel et al., 2010; Abetz et al., 2006; Sijbesma et al.,
2008).
Important progress has been achieved and relevant experience
obtained in the past by testing membrane modules in real ue
gas environments. In Europe, under the framework of the projects
MemBrain (MEM-BRAIN Alliance, 2011), METPORE (METPORE,
2014), Nanoglowa (CO2 Capture Using Membrane Technology,
2015) and iCap (The iCap project), different polymer and ceramic
membranes are being investigated to meet the harsh requirements
in coal-red power plants (Car et al., 2008a; Hussain and Hgg,
2010; Brinkmann et al., 2011; Reijerkerk et al., 2010; Bram et al.,
2011). Membrane modules equipped with Polyactive thin-lm
composite membranes (Car et al., 2008c; Brinkmann et al., 2013;
Brinkmann et al., 2012; Brinkmann et al., 2010) in a parallel con-
guration (12.5 m2 and 1 m2 ) are currently being tested in the
EnBW power plant Rheinhafen-Dampfkraftwerk (Bram et al., 2011;
METPORE, 2014). A 1 MWel pilot-scale Polaris membrane separa-
tion system at the Department of Energys National Carbon Capture
Center in Wilsonville, USA, was announced by the National Energy
Technology Laboratory (NETL) in November 2012. It will test a post-
combustion membrane capture technology on the largest scale in
the world to date (Merkel et al., 2010; NETL Greenlights 1 MW Field
Test For Membrane Capture Tech, 2012).
In order to realize the potential of gas permeation for industrial
applications, advanced membrane module concepts are desirable.
Membranes can be inserted into three major types of modules
for gas separation applications: envelope-type, spiral wound, and
hollow ber modules (Favre, 2010; Melin and Rautenbach, 2003;
Baker, 2012; Ohlrogge and Wind Brinkmann, 2010). In general,
the membrane module must be used in commercial processes as
a package with as much surface area per unit volume as possi-
ble, good ow distribution and efcient contact of the feed gas
within the membrane. The main ow congurations in membrane
196 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204
Table 1
Packing density range of different membrane module forms (Favre E., 2010).
Module form PD [m2 /m3 ]
Hollow ber 20005000
Spiral wound 7001000
Envelope module 500900
gas permeation processes are cross-plug ow, co-current ow and
counter-current ow (Melin and Rautenbach, 2003). More specif-
ically, hollow ber modules may be designed with reasonable
precision to approximate an idealized counter-current when the
permeate pressure is signicant, or to approximate a cross-ow
pattern when the permeate pressure is low enough (Favre, 2010).
The most commonly used at sheet membrane module for gas sep-
aration is the spiral wound module, which is dominated by cross
ow (Merkel et al., 2010). Within an envelope-type module, the rst
half of a membrane envelope can be assumed to be in co-current
ow conguration, whilst the second half is in counter-current ow
conguration (Brinkmann et al., 2013). The packing density (PD)
of each type of membrane, which is the surface area per volume
[m2 /m3 ], is shown in Table 1. Furthermore, the ow patterns do not
only inuence the concentration distribution on the feed and per-
meate sides of the module but also give rise to different behavior in
terms of pressure drops (Melin and Rautenbach, 2003; Brinkmann,
2006) and hence the utilization of the available driving force.
Although hollow ber modules appear to be superior in terms
of membrane area utilization, they have substantial drawbacks
when high-ux membrane materials are employed in a thin-lm
composite conguration. In order to transfer the attractive CO2 /N2
selectivities at 20 C of approx. 60 of poly(ethylene oxide) block
copolymers as Polyactive or Pebax 1657 (Car et al., 2008c,b)
into a membrane module, whilst also achieving high CO2 perme-
ances in the order of 3 Nm3 / (m2 h bar) at 20 C, ultrathin layers
with a thickness in the order of 70 nm are required. This ambi-
tious goal can be met by manufacturing at sheet membranes on
a 100 m2 scale (Brinkmann et al., 2012). To the authors knowl-
edge, no comparable coating technology is available for hollow ber
membranes. In the present work, different ow patterns will be
investigated in at sheet membrane modules within the frame-
work of the METPORE II project (METPORE, 2014; Brinkmann et al.,
2013). The envelope-type modules used in our experiments were
developed by Helmholtz-Zentrum Geesthacht (HZG) (Brinkmann
et al., 2013; Baker, 2012; Ohlrogge et al., 2006). They were tested
both on a pilot plant scale and in the ue gas of the power plant
Rheinhafen-Dampfkraftwerk (EnBW). The pressure drop in the
modules was investigated. The relevant results were integrated
in a total system analysis using ue gas data from the Reference
Power Plant North Rhine-Westphalia (RKW-NRW) (Konzeptstudie:
Referenzkraftwerk Nordrhein-Westfalen (RKW NRW), 2004). The
equation-oriented process simulator Aspen Custom Modeler1 was
used for membrane module simulation. The cascaded membrane
process was investigated by Aspen Process Modeling V8.0.
2. Investigation of pressure distribution in a at sheet
membrane module (Brinkmann et al., 2013)
2.1. Introduction of membrane material and module
The membrane considered in this study is a multilayer, thin-lm
composite membrane specically developed for the separation of
CO2 from N2 . Details on this membrane can be found in (Car et al.,
1
http://www.aspentech.com/products/aspen-custom-modeler.aspx, last access
on 27th June 2014.
Table 2
Free-Volume parameters for Polyactive composite membrane (Brinkmann et al.,
2013).
L0 [Nm3 /(m2 h bar)] E [kJ/kmol] m0 [1/bar] mT [1/K]  []
CO2 1084.66 14279.81 0.1568 -0.0054 3.941
N2 68646.60 34251.30 0.0000 0.0000 3.798
O2 39776.50 30463.00 0.0000 0.0000 3.467
2008c; Brinkmann et al., 2013, 2012, 2010; Metz et al., 2005b).
The 70 nm thin separation layer consists of the polyethylene /poly-
butylteraphtalate block copolymer Polyactive . The active layer is
sandwiched between two highly permeable polydimethylsiloxane
layers cast in turn onto a porous support structure consisting of
polyacrylonitrile and polyester. The CO2 permeance and the CO2 /N2
selectivity of this membrane are similar to the published values
for the MTR Polaris membrane (Lin et al., 2014). The Polyactive
membrane used here has been extensively tested for applications
as diverse as biogas processing (Brinkmann et al., 2012, 2010),
separation of CO2 from reaction products (Stnkel et al., 2011;
Song et al., 2013) and ue gas treatment (Brinkmann et al., 2013,
2012). The relevant permeation properties are given in Table 2, in
which L0 is the permeance for T and p 0, E is the activa-
tion energy, m0 and mT are free-volume model parameters, and 
is the Lennard-Jones molecule diameter. Only CO2 , N2 and O2 are
listed. The permeance of Ar was assumed to be identical to that of
O2 whilst that of H2 O was assumed to be ten times the value of
that for CO2 . The parameters are given for the free-volume model
(Brinkmann et al., 2013; Fang et al., 1975; Alpers, 1997) which
has been employed to express multicomponent permeation behav-
ior in modeling. The parameters were determined using single-gas
measurements employing the pressure increase method. The mem-
brane was produced on a 100 m2 scale and was installed in different
module types, mostly into envelope-type modules.
These modules had a maximum capacity of 75 m2 with a length
of 1250 mm and a diameter of 310 mm, depending on envelope
thickness. The membrane material was manufactured into mem-
brane envelopes consisting of two sheets of membrane material
with their separation layer on the outside and a permeate spacer
between the sheets. They were thermally welded at the outer
circumference. The permeate was withdrawn radially toward a
central hole. The membrane envelopes were stacked on a per-
forated permeate tube and subdivided into compartments, thus
allowing the cross-sectional area to be adjusted depending on the
amount of permeate withdrawn. Hence, a nearly constant ow
velocity on the feed side could be realized. More details on this
module type can be found in (Brinkmann et al., 2013; Ohlrogge and
Wind Brinkmann, 2010; Ohlrogge et al., 2006). The spiral wound
membrane module is widely used in membrane technology, and
its design features are outlined in (Baker, 2012). A novel concept
for at sheet membranes is closely related to the envelope type
(Brinkmann et al., 2011; Brinkmann et al., 2013, 2012) but the
envelopes are rectangular and are housed in a module with a rect-
angular cross section. The design allows for different points of
permeate withdrawal so that different ow patterns can be real-
ized, i.e. co- and counter-current design. Furthermore, it is possible
to divide the envelope into segments, thus realizing different per-
meate withdrawal points along the ow path from the feed to the
retentate, hence minimizing the pressure drop on the permeate
side. Fig. 1 illustrates the investigated module types.
2.2. Test equipment
The envelope-type module has been extensively studied in pilot
plant investigations for the separation of CO2 from various gas
streams using Polyactive membranes (Brinkmann et al., 2011,
 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204 197

Fig. 2. Gas permeation pilot plant for power plant ue gas installed at EnBW Rheinhafen-Dampfkraftwerk, Karlsruhe, Germany.

Table 3
Experimental conditions of the pilot plant experiments using synthetic gas mixtures and experimentally determined as well as simulated retentate pressures at a temperature
of 20 C for an envelope type membrane module containing 9.52 m2 of Polyactive membrane (Brinkmann et al., 2013).

Experiment no. Feed volumetric Feed pressure Permeate pressure Feed CO2 mole Retentate Pressure [bar]
owrate [Nm3 /h] [bar] [bar] fraction []
Experiment Simulation

1 43.64 4.41 0.20087 0.181 4.34 4.33

2 44.41 4.48 0.111 0.177 4.41 4.40
3 36.00 4.38 0.099 0.180 4.33 4.32
4 26.31 4.32 0.095 0.182 4.29 4.28
5 34.24 2.55 0.201 0.174 2.45 2.45
6 33.64 2.49 0.100 0.176 2.40 2.39
7 20.07 2.52 0.101 0.182 2.48 2.48
8 42.61 4.44 0.200 0.167 4.36 4.36

2013, 2012, 2010). It is employed in numerous industrial applica-
tions in the chemical and petrochemical industries (Ohlrogge and
Wind Brinkmann, 2010; Ohlrogge et al., 2006, 2005). The analysis
of different module types presented in (Brinkmann et al., 2013) was
constrained to two applications. In addition to synthetic gas mix-
tures, a bypass stream from the Rheinhafen-Dampfkraftwerk was
supplied to a dedicated pilot plant within the scope of the project
METPORE II, which was funded by the German Ministry of Eco-
nomics and Energy. A simplied ow sheet is shown in Fig. 2. A
separate publication describing its design and the results achieved
in detail is in preparation (Pohlmann and Brinkmann, 2014).
simulation results closely reect the experimental values. The pre-
diction of the separation performance is equally good (Brinkmann
et al., 2013). The relevant results for pressure drops employing real
ue gas at the EnBW Rheinhafen-Dampfkraftwerk are shown in
Table 4. The accuracy of the model predictions allows the developed
models to be applied for the estimation of the required compression
energies.
2.4. Simulation of different module types in a virtual pilot plant
conguration

Fig. 3 illustrates a possible pilot plant system. A feed ow of

2.3. Modeling validation
The permeation behavior of multicomponent mixtures through
Polyactive multilayer composite membranes can be described by
the free-volume model using the parameters given in Table 2. In
(Brinkmann et al., 2013; Brinkmann, 2006), it was shown that the
combination of this model with an appropriate model describing
the membrane module ow patterns can very accurately pre-
dict the separation performance of envelope-type modules. It was
assumed that this is also true for the other membrane module types
considered here. However, it should be emphasized that this has yet
to be experimentally veried. The details of the models employed
here can also be found in (Brinkmann et al., 2013). They were imple-
mented in the equation-oriented process simulator Aspen Custom
Modeler (ACM).1 The operating conditions investigated in the pilot
plant as well as the experimental and simulation results for the
retentate pressure are summarized in Table 3. It is apparent that the
1000 Nm3 /h was assumed to enable the investigation of membrane
modules commonly employed in todays gas permeation installa-
tions. The blower C1 was used to compensate the pressure drops of
the membrane modules installed in the rst stage of the process,
i.e., the retentate pressure was set to atmospheric pressure and the
outlet pressure of C1 was adjusted according to the pressure drop.
The simulation assumed adiabatic compression with an efciency
of 70%. The cooler H1 was used to cool the feed gas to 25 C and to
separate condensed water whilst the heater H2 increased the feed
temperature above the dew point in order to prevent condensation
in the downstream system. The membrane modules in MemStage1
separated CO2 from the feed gas according to the set recovery tar-
get, i.e., the CO2 separation degree, which was assumed to be 50%
for this investigation. The vacuum pump C2 compressed the per-
meate of the rst stage. Its suction pressure was set to 100 mbar.
Since water preferentially permeates the membrane, i.e., even more
strongly than CO2 , the separator S1 was employed to draw off the
198 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204

Table 4
Experimental conditions of the pilot plant experiments using ue gas and experimentally determined as well as simulated retentate pressures at temperatures of 2428 C
for an envelope type membrane module containing 12.5 m2 of Polyactive membrane.

Experiment no. Feed volumetric Feed pressure Permeate pressure Feed CO2 mole Retentate Pressure [bar]
owrate [Nm3 /h] [bar] [bar] fraction []
Experiment Simulation

1 50.00 1.13 0.060 0.135 1.10 1.09

2 50.30 1.14 0.062 0.130 1.11 1.11
3 60.20 1.18 0.063 0.135 1.14 1.13
4 69.90 1.24 0.057 0.135 1.19 1.19
5 80.00 1.31 0.062 0.129 1.25 1.25
6 50.30 1.14 0.075 0.129 1.11 1.11
7 59.70 1.19 0.066 0.131 1.15 1.15
8 65.00 1.22 0.075 0.128 1.18 1.17
9 69.60 1.23 0.065 0.136 1.18 1.18
10 70.40 1.25 0.069 0.129 1.20 1.19
11 79.60 1.29 0.067 0.138 1.22 1.23
12 80.10 1.31 0.069 0.130 1.25 1.25
13 80.10 1.31 0.069 0.135 1.25 1.25
14 80.30 1.30 0.067 0.136 1.24 1.24
15 80.60 1.31 0.069 0.136 1.25 1.25
16 60.30 1.20 0.111 0.128 1.16 1.15
17 79.70 1.32 0.116 0.129 1.25 1.26
18 80.00 1.31 0.100 0.137 1.25 1.25
19 80.30 1.32 0.100 0.132 1.25 1.26
20 60.00 1.20 0.150 0.128 1.16 1.16
21 70.00 1.26 0.151 0.131 1.20 1.21
22 80.00 1.32 0.150 0.128 1.26 1.26

Fig. 3. Pilot plant ow sheet.

liquid water. The vacuum pump was assumed to operate isother-
mally with an efciency of 40%, as can be realized by liquid ring
vacuum pumps. In operation, this lower efciency was offset by a
simple, robust design, the partial condensation of permeated water
in the service liquid circuit and a lower demand of cooling utili-
ties since the heat of compression was transferred to the service
liquid which was cooled down in a straightforward fashion. The
adiabatic compressor C3 increased the pressure to 6 bar, i.e., the
operating pressure of the second stage, at an efciency of 70%. The
heat exchanger H3 cooled down the gas and removed the liqueed
water. The membrane stage MemStage2 was employed to further
increase the CO2 concentration of the permeate stream of Mem-
Stage1 to the required purity, i.e., 95 vol%, in the permeate of the
second membrane stage at a pressure of 1.0130 bar. In order to
achieve the required recovery, the retentate was recycled upstream
of H1. Part of the compression energy was recovered by the turbo
expander T1 (efciency 70%).
For comparison, the required membrane areas were calculated
for the described separation task (i.e., a CO2 purity of 95 vol% at a
CO2 separation degree of 50 %). It was assumed that the membrane
stages could be described as cross-ow stages with unhindered per-
meate withdrawal and no pressure drops on the feed or permeate
side as well as no concentration polarization. The dependency of the
permeances on temperature, pressure and composition was con-
sidered as well as real gas behavior for the calculation of the driving
forces and non-isothermal operation due to the JouleThomson
effect. The latter two phenomena were of minor effect, especially in
the rst stage, due to the low pressures and the small stage cut. The
simulation rendered area requirements of 300 m2 for stage 1 and
8.2 m2 for stage 2. Using these area requirements, at sheet mem-
brane modules were dimensioned for both stages. The following
module types were considered (see also Fig. 1):
Envelope-type membrane module.
Spiral wound membrane module.
Counter-current membrane module concept with one segment.
The permeate was led counter-currently to the feed ow and
withdrawn at the feed side of the module.
Co-current membrane module concept with one segment where
the permeate was withdrawn co-currently with the feed at the
retentate location.
Counter-current membrane module concept with four segments.
The module was divided into four sections of equal length, and
at the start of each segment, permeate was withdrawn at the
location of the feed.
 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204 199

Table 5
Membrane module details stage 1.

Envelope Spiral wound Counter-current Co-current Counter-current 4 segments

Membrane area per module A [m2 ] 60.21 20.11 300.72 300.72 300.72
Number of modules in parallel 5 8 and 7 1 1 1
Module diameter D [m] 0.310 0.203
Number of envelopes 506 11 127 127 127
Compartments 9
Envelope breadth b [m] 0.914 0.600 0.600 0.600
Envelope length l [m] 1.000 1.973 1.973 4 0.493
Feed channel height hR [mm] 1.500 1.500 1.500 1.500 1.500
Permeate channel height hP [mm] 1.500 1.500 1.500 1.500 1.500

Table 6
Membrane module details stage 2.

Envelope Spiral wound Counter-current Co-current Counter-current 4 segments

Membrane area A [m2 ] 8.33 8.33 8.21 8.21 8.21

Number of modules in parallel 1 1 1 1 1
Module diameter D [m] 0.310 0.159
Number of envelopes 70 9 5 5 5
Compartments 22
Envelope breadth b [m] 0.693 0.300 0.300 0.300
Envelope length l [m] 0.668 2.736 2.736 4 0.684
Feed channel height hR [mm] 1.500 1.500 1.500 1.500 1.500
Permeate channel height hP [mm] 1.500 1.500 1.500 1.500 1.500

In addition to the previously described phenomena, pressure

drops were considered on the feed and permeate sides, as well as
concentration polarization on the feed side. Details on the simu-
lation models employed, their implementation in Aspen Custom
Modeler1 and the employed geometrical values can be found else-
where (Brinkmann et al., 2013). Tables 5 and 6 show the module
details required for the simulation of stages 1 and 2, respectively. All
membrane modules are assumed to be equipped with a Polyactive
membrane (Car et al., 2008c; Brinkmann et al., 2013, 2012). For the
co- and counter-current membrane module concepts, one mem-
brane module can be used for each of the stages, since this concept
is quite versatile in terms of adjusting it for different ow rates.
However, an important point to mention is that the simulation
predictions for this module type have not yet been validated exper-
imentally. For the envelope-type and spiral wound modules, it
was assumed that ve or eight modules were mounted in paral-
lel in the rst stage, respectively. In the case of the spiral wound Fig. 4. Pressures on the retentate/feed side and permeate side in the different mod-
modules, a second sequential set of seven parallel modules was ule types.
required to realize the required membrane area. For the second
stage, one membrane module was sufcient for both envelope and
spiral wound module types.
The results of the simulations are summarized in Table 7 and
Figs. 46. Since stage 1 governs the process, the discussion will
focus on this stage. The differences in pressure drops for the inves-
tigated modules are rather small, as shown in Fig. 4. It is apparent
that both the non-segmented counter-current and the co-current
modules have the highest pressure drops on the permeate side and
low pressure drops on the feed side. The latter is also true for the
four-segment counter-current concept. However, due to the seg-
mentation, low pressure drops can also occur on the permeate side.
This causes a superior pressure ratio (Fig. 5) and a good CO2 driving
force (Fig. 6). The pressure on the permeate side of the spiral wound
modules is quite high. This is due to the long permeate pathways.
High pressure drops also cause the high pressures on the feed side.
In combination, these factors lead to a good pressure ratio and a
good driving force (Figs. 5 and 6). The module with the best uid
dynamics is the envelope-type module. It has very short perme-
ate pathways resulting in small pressure drops on the permeate
side (Fig. 4). Using the calculated performance data for the differ-
ent modules to compare CO2 purities and recoveries, as well as the Fig. 5. Pressure ratios of the different module types.
required power for the blower C1, the vacuum pump C2 and the
200 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204

Table 7
Simulation results.

Envelope Type Spiral Wound Counter-Current 1 Segment Co-Current Counter-Current 4 Segments

CO2 -purity [kmol/kmol] 0.944 0.943 0.946 0.932 0.945

CO2 -recovery [] 0.451 0.451 0.431 0.401 0.455
Membrane area stage 1 [m2 ] 301.070 301.620 300.716 300.716 300.716
Membrane area stage 2 [m2 ] 8.330 8.330 8.207 8.207 8.207
Total membrane area [m2 ] 309.400 309.950 308.923 308.923 308.923
Power blower C1 [kW] 7.991 9.260 7.260 7.296 7.262
Power vacuum pump C2 [kW] 17.674 17.875 17.782 15.902 17.751
Power compressor C3 [kW] 9.016 9.177 8.769 8.320 8.940
Power turbine T1 [kW] 0.933 0.985 0.952 0.928 0.927
Total power [kW] 33.748 35.326 32.859 30.592 33.026
Total cooling duty [kW] 137.607 139.318 136.351 135.971 136.623
Pressure drop stage 1 retentate [bar] 0.092 0.120 0.076 0.077 0.076
Max. pressure drop stage 1 permeate [bar] 0.0002 0.0088 0.0118 0.0152 0.0008
Pressure drop stage 2 retentate [bar] 0.340 0.005 0.088 0.084 0.089
Max. pressure drop stage 2 permeate [bar] 0.0015 0.0318 0.1638 0.2545 0.0152
Permeate owrate stage 1 [Nm3 /h] 97.901 98.990 98.500 88.040 98.300

lar behavior. It was employed to recompress the permeate from

stage 1 before feeding it to stage 2. Since envelope-type and spiral
wound modules had the highest pressure drops on the feed side
the blower powers were also higher for these modules with con-
sumption being the highest for the spiral wound module. This was
due to the high velocity on the feed side, i.e., 2.5 m/s, compared to
ca. 2 m/s for the other modules. This high velocity resulted from
distributing modules of a given area and geometry to achieve the
required membrane area.
It can be concluded that the segmented counter-current mem-
brane module appears to be the best choice in terms of CO2 purity
and recovery, as well as energy consumption of the rotating equip-
ment.

3. Power-plant data used for simulation

A scaled-up cascaded membrane system, shown in Fig. 7, was

Fig. 6. CO2 driving forces of the different module types.
compressor C3, it is apparent that the segmented counter-current
module renders the highest CO2 purity with the highest recovery.
The envelope-type and spiral wound modules are close contenders.
Considering the one-segment co- and counter-current modules, the
situation regarding CO2 recovery is more pronounced: recovery is
strongly decreased, especially for the co-current module. This is
due to the inferior pressure ratio and driving force distribution in
these module types (Figs. 5 and 6). In terms of compression power
consumption, the highest demand is caused by the vacuum pump
C2 followed by the compressor C3 and the blower C1. The low-
est power demand for the vacuum pump was observed for the
co-current module, which had the lowest permeate ow rate due
to its inferior driving force utilization. In other words, the vacuum
pump power follows the permeate ow rate to be withdrawn from
stage 1. The power demand of the compressor C3 showed simi-
used for the process analysis. The rst membrane (Mem 1) was
driven by a vacuum pump and the second membrane (Mem 2) by a
compressor. The retentate of the second membrane was recycled as
the feed of the rst membrane. Part of the compression energy was
recovered by a turbo expander. The membrane cascade was located
downstream of the SCR-DeNOx, dust removal (E-lter) and desul-
phurization (FGD) processes and prior to the cooling tower. Here,
the ue gas had a pressure of approximately 1 atm and a tempera-
ture of 5070 C. The basic data of RKW-NRW and the ue gas data
are listed in Table 8. The ue gas data were obtained by simulation
using Klein Kopje hard coal. The residue of pollutants in the ue
gas consisted of approximately 50 vppm SO2 and approximately
200 vppm NO2 .
The temperature, H2 O permeance and relative humidity had an
evident inuence on the CO2 selectivity of polymer membranes
(Low et al., 2013). In order to develop a feasible membrane system,
these inuence factors must be considered.

Fig. 7. Schematic illustration of the scaled-up cascaded membrane system.

 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204 201

A wet scrubber was adopted upstream of the membrane system,

referring to a post-combustion process presented by RWE (Peters
and Wallus, 2012). This scrubber had two functions: the rst was
to further reduce the pollutants (SOx, NOx and dust) in the ue gas,
e.g., SOx can be decreased to 10 vppm; the second was to cool the
ue gas down further to 2530 C. The latter function is a crucial
factor for the membrane process, because the working temperature
of the Polyactive membrane inuences its performance strongly
(Zhao et al., 2013). Furthermore, applying a dewatering process
prior to CO2 separation leads to a lower energy consumption of
the whole system (Zhao et al., 2013). Here, 2/3 water content of the
ue gas was removed.

4. Integrating the module data with the scaled-up cascaded

membrane system

4.1. Simulation of single-stage system

In order to investigate the inuence of ow patterns on mem-

brane separation performance, a case study was carried out. Two
different cases were explored with a feed ow rate of 100 kmol/h,
composition of 14.91 mol% CO2 , 0.59 mol% H2 O and 84.50 mol% N2 ,
membrane CO2 permeance of 3 Nm3 /(m2 h bar), CO2 /N2 selectivity
of 50, H2 O permeance of 30 Nm3 /(m2 h bar). Case 1 had a feed pres-
sure of 4 bar and a permeate pressure of 0.1 bar; case 2 had a feed
pressure of 1 bar and a permeate pressure of 0.1 bar. The results are
shown in Fig. 8(a) and (b), respectively. The working temperature
of the membranes was 25 C.
Comparing these two diagrams, it is apparent that using both
compressor and vacuum pump for a membrane leads to a smaller
membrane area. In case 1, co-current ow had a slightly better CO2
purity than cross- and counter-ow at a low CO2 separation degree
(<60%). In case 2, the CO2 purity attenuated intensely when the CO2
separation degree exceeded 40%; co-current ow showed a strong
decrease in CO2 purity when the CO2 separation degree exceeded
40%, because of a decreased CO2 driving force caused by the simul- Fig. 8. Polyactive membrane performance for different ow patterns: (a) feed
taneous decrease in CO2 content on the feed side and increase on pressure 4 bar, permeate pressure 0.1 bar, membrane area = 1 m2 , 51 m2 , 101 m2 ,
the permeate side. 1000 m2 ; (b) feed pressure 1 bar, permeate pressure 0.1 bar, membrane area = 1 m2 ,
51 m2 , 101 m2 , 10,000 m2 .

Table 8 4.2. Simulation of the scaled-up cascaded system

RKW-NRW power plant basic data and simulation results of the ue gas conditions
after removal of the pollutants using Klein Kopje hard coal (Zhao et al., 2013).
Using the system shown in Fig. 7, three ow patterns were
Power plant RKW-NRW investigated in the platform of the NRW reference power plant.
Output gross 600 MW A detailed description of the system can be found in our previ-
Output net 555 MW ous paper (Zhao et al., 2012). The feed ue-gas composition and
Net efciency 45.9% conditions are listed in Table 8. O2 /N2 and Ar/N2 selectivity were
Steam parameters 285 bar/ 600 C / 620 C assumed to be 2.8. The captured CO2 was compressed to 110 bar at
Operating time 8000 h/year
Fuel input 1.33 Mt/year
30 C. In the study, the Peng Robinson cubic equation of state with
Investment costs 534.4 million euro the BostonMathias alpha function (PR-BM) was applied as imple-
O & M costs 7.8 million euro/year mented in Aspen Process Engineering. The polytropic efciency of
Fuel costs 72.8 euro/t the compressors, expanders and vacuum pumps was assumed to
Electricity price 4.355 cent/kWh
be 85%. A two-stage vacuum pump was used in the simulation for
Flue gas conditions after removal of the pollutants Mem 1, a two-stage compressor for Mem 2 and an eight-stage com-
Pressure 1.05 bar pressor for CO2 compression processes. A pressure drop of 30 mbar
Temperature 50 C
was considered in each intercooler. The simulation results of the
Flow rate 1.6 million Nm3 /h
three different ow patterns are presented in Table 9.
Main components
The separation target of the system was dened as 95.0 mol%
CO2 13.5 mol%a
N2 70.1 mol%a
CO2 purity after CO2 compression, CO2 separation degrees of 50.0%
O2 3.7 mol%a and 70.0 %, H2 O content of 500 vppm. The optimization target of
H2 O 11.9 mol%a the system was minimum energy consumption. Membrane areas
Ar 0.8 mol%a of Mem 1 and 2 were the two variables which were regulated in
a
simulated. the simulation to reach the desired separation target.
202 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204

Table 9
Inuence of ow patterns on the scale-up cascaded system.

Flow CO2 purity Degree of CO2 Membrane area Specic energy Efciency loss
pat- [mol%] separation [km2 ] consumption [%-pts.]
terns [%] [kWh/tseparatedCO2 ]
Mem 1 Mem 2

Cross 95.0 70.0 1.83 0.05 243.8 5.9

95.0 50.0 0.85 0.04 217.3 3.8
Co-current 93.8 60.0 1.83 0.05 254.8 5.3
95.2 55.3 1.52 0.05 243.5 4.8
95.0 50.0 1.04 0.04 229.1 4.0
Counter-current 95.0 70.0 1.52 0.05 229.5 5.6
95.0 50.0 0.79 0.04 213.2 3.7

For a CO2 separation degree of 50%, the aforementioned separa-

tion target was easy to achieve. The results in Table 9 indicate that
the counter-current module consumed the lowest specic energy
of 213.2kWh/tseparatedCO2 with an efciency loss of 3.7% points.
For a CO2 separation degree of 70%, it was unproblematic for
cross- or counter-current ow setups to reach the dened separa-
tion target. However, for the co-current module, the program could
not converge, i.e., the co-current cascaded system could not reach
95 mol% CO2 purity and a CO2 separation degree of 70% simultane-
ously. It is well known that Mem 1 dominates the systems overall
separation performance depending on the CO2 separation degree
(Zhao et al., 2012, 2008). Fig. 8(b) shows that a co-current module
approaches its upper limits with a CO2 separation degree of 70%.
This caused the convergence problems of the system. Hence, for
the co-current module, a specication design was carried out, i.e.,
membrane areas of the two membranes were given as input; the
CO2 purity and CO2 separation degree were calculated. The results
Fig. 9. Additional compression energy against pressure drops in different mem-
for the membrane area data of cross and counter-current ows at brane modules at a CO2 separation degree of 50%.
a CO2 separation degree of 70% are shown in Table 9.
One point to be highlighted here is that using real ue gas for
the scaled-up cascaded system led to a lower energy consumption
and smaller membrane areas in comparison with the system using
ideal ue gas (14 mol% CO2 and 86 mol% N2 ) (Franz et al., 2013).
The reason for this is that H2 O functions as a sweep gas, since it
more readily permeates than CO2 . This sweep effect contributes to
a lower area requirement and a lower specic energy. Furthermore,
counter-current ow was more advantageous in terms of energy
consumption and membrane area requirement.

4.3. Inuence of pressure drop in the membrane module on the

total system energetic consumption

In order to compensate the pressure drop in the membrane

module, additional compression energy was applied. The sim-
ulation results for three ow patterns are listed in Table 10.
Furthermore, the required additional energy both at the retentate
and permeate side was calculated for a CO2 separation degree of
50%, which is represented by a bar chart in Fig. 9.
The results reveal that the lowest additional specic energy
was needed for the counter-current module, owing to the lower Fig. 10. Comparison of efciency loss for different ow patterns with chemical
absorption.
pressure drop at the retentate side. The pressure drop at the reten-
tate side in the rst membrane dominates the overall compression
energy. In the virtual pilot plant conguration investigations
counter-current ow, respectively. Pressure drop (pd) is indicated
(Section 2.4), the vacuum pump power demand played a more
by a dashed line with crossed symbol.
pronounced role due of the assumption of low efciency, which
One point to be emphasized here is that chemical absorption has
is typical for liquid ring machines.
also become the subject of intense development over the past few
years. Some new solvents, e.g., Gustav 200 and Ludwig 540 (Peters
4.4. Comparison with chemical absorption and Wallus, 2012), are synthesized with a lower energy demand
(approximate 2700MJth /tCO2 ) for regeneration processes (shown
Membrane capture and chemical absorption were compared in Fig. 11).
and the results are depicted in Fig. 10. The hollow square, cir- The results show that counter-current ow exhibits the best
cle and triangle with solid lines represent cross, co-current and performance in comparison with the other module forms when the
 T. Brinkmann et al. / International Journal of Greenhouse Gas Control 39 (2015) 194204 203

Table 10
Integrating the pressure drop of different modules with the scale-up cascaded membrane system.

Module type Degree of CO2 purity Pressure Pressure Pressure Pressure Additional Additional
CO2 [mol%] drop at drop at drop at drop at specic efciency
separation Mem 1 Mem 1 Mem2 Mem 1 energy loss
[%] retentate permeate retentate permeate consumption [%-pts.]
side [bar] side [bar] side [bar] side [bar] [kWh/tseparatedCO2 ]

Cross 70.0 95.0 0.12 0.0088 0.005 0.0318 26.0 0.63

50.0 95.0 0.12 0.0088 0.005 0.0318 32.4 0.56
Co-current 60.0 93.8 0.077 0.0152 0.084 0.2545 28.3 0.59
50.0 95.0 0.077 0.0152 0.084 0.2545 29.5 0.51
Counter- 70.0 95.0 0.076 0.0118 0.088 0.1638 21.5 0.52
current 50.0 95.0 0.076 0.0118 0.088 0.1638 25.6 0.45

aforementioned types. For the co-current module, this is even more

pronounced, as the high pressure drop is combined with a disad-
vantageous ow pattern leading to both low purity and recovery.
This leads in turn to lower compression energies in the vacuum
pump and in the recycle compressor. However, it is unlikely that
this will offset the inferior performance of the module.
If a CO2 purity of 95% is aspired to, membranes are especially
advantageous if CO2 separation degrees of up to 70% are the aim.
In this case, the efciency losses are in the range of 46%, which
is lower than related efciency losses of MEA absorption even if
new solvents are applied. For the scaled-up cascaded membrane
system simulation, the counter-current module shows the best per-
formance in comparison with the other module types. It has the
smallest membrane area and the lowest energy consumption.
Fig. 11. Energy demand for new solvents and an optimized MEA process (Peters
and Wallus, 2012).
Acknowledgements

pressure drop is considered in the module. Counter-current ow
also leads to a better output than the chemical solvents.
5. Conclusions
Financial support from the METPORE II project (funding identi-
er: 03ET2016), funded by the German Ministry of Economics and
Energy (BMWi), Germany, within the framework of the COORETEC
program, is gratefully acknowledged.

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