Research Article 1675

Abulhassan Ali
Energy Minimization in Cryogenic Packed
Khuram Maqsood
Nor Syahera Beds during Purification of Natural Gas with
Azmi B. M. Shariff
High CO2 Content
Saibal Ganguly

Universiti Teknologi PETRONAS,
Chemical Engineering
Department, Perak, Malaysia.
Minimization of energy consumption was explored for countercurrent switched
cryogenic packed beds in which separation of CO2 and other components of natu-
ral gas can be achieved based on differences in freezing or desublimation points.
Highly pure CO2 and methane were obtained after separation. An experimental
setup for CO2 removal from natural gas was constructed and a detailed experi-
mental study was conducted by changing different operating parameters. Com-
pared to other cocurrent or jacket-cooled constant-temperature configurations,
countercurrent switched beds provided optimal separation and energy efficiencies.
The effects of important process parameters like initial temperature profiles of the
cryogenic bed, feed composition, and feed flow rate on energy requirement, bed
saturation, bed pressure, and cycling times were investigated. The energy
requirement for cryogenic packed beds was compared with the conventional cryo-
genic distillation process.

Keywords: CO2 removal, Cryogenic CO2 capture, Cryogenic packed bed, Energy minimization,
Natural gas
Received: April 27, 2014; revised: May 28, 2014; accepted: July 22, 2014
DOI: 10.1002/ceat.201400215

1 Introduction In 2002, Clodic and Younes [3, 4] developed a cryogenic CO2

Natural gas is a fossil fuel, which is the cleanest primary energy
source of the world. Raw natural gas essentially requires pro-
cessing to remove impurities in order to meet the market speci-
fications. The huge market demand for natural gas has led to
the exploration of high impurity wells worldwide. Though sev-
eral impurities are present in Malaysian natural gas, the high
content of CO2, i.e., up to 80 %, not only causes corrosion of
piping and process equipment, it also decreases the calorific
value of natural gas [1].
The technologies of CO2 separation mainly comprise of
absorption, adsorption, membrane separation, and cryogenic
separation [2]. The cryogenic separation technology has been
known for several decades. However, this technology was not
extensively studied due to the common perception of high
expected cooling duty. Cryogenic separation involves no chem-
ical reaction and CO2 can be captured at high pressure as well
as atmospheric pressure. With these advantages, the research
on cryogenic CO2 removal technologies has recently gained
significant momentum.
– both H2O and CO2 were desublimated at different locations of
Correspondence: Prof. Dr. Saibal Ganguly (gangulysaibal2011@gmail.
com), Universiti Teknologi PETRONAS, Chemical Engineering
Department, Bandar Sri Iskandar, 31750, Perak, Malaysia.
capture process. CO2 desublimated as a solid on the surfaces of
heat exchangers, which were cooled by evaporating a blend of
refrigerants. The energy required for this process was reported
in the range of 541–1119 kJ kg1 CO2 . The limitations of this pro-
cess are prior removal of water in order to avoid plugging.
In 2010, Tuinier et al. [5, 6] developed a novel cryogenic CO2
capture process using dynamically operated packed beds. This
process comprised of three cycles: (a) cooling, (b) capture, and
(c) removal. In the cooling cycle, the packing in the bed was
brought below the freezing temperature of CO2 and then in
capture cycle flue gases were introduced. Using refrigerated
beds at atmospheric pressure, an effective separation between
H2O, CO2, and the permanent gases was obtained; 99 % CO2
was recovered from a flue gas containing 10 vol % CO2 and
1 vol % H2O. The energy required for this process was 1.8 MJ
kg1
CO2 . A simulation study on CO2 separation from biogas has
been reported by Tuinier et al. [7]. The disadvantages of this
process are that it is yet to be tested on natural gas and mix-
tures of hydrocarbons at higher pressures and very high CO2
concentrations.
In 2011, Chun-Fang et al. [8] proposed a new process to cap-
ture CO2 from flue gases using Stirling coolers. In this process,
the capture setup and the permanent gas flows out without any
phase change. Up to 96 % of CO2 could be recovered in this
process. Energy required for this process was reported to be
1.5 MJ kg1
CO2 . In 2012, Yang and Xu developed a systematic

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1676 Research Article

methodology for minimization of product loss of an integrated Table 1. Physical properties of the cryogenic packed bed.
cryogenic separation system [9].
Most processes described in literature involve CO2 capture Length of bed 0.46 m
from flue gases. However, the application of desublimation to Diameter of bed 0.0418 m
the natural gas is hardly available in the existing literature. Fur-
thermore, the concentration of feed CO2 used in the previous Diameter of packing 0.01m
studies is very low compared to CO2 contents present in Density of packing 2562 kg m–3
Malaysian natural gas. Also, the engineering aspects of changes
in feed concentrations, feed temperatures, bed temperature Porosity eg 0.637
profiles, desublimation packed-bed configurations like cocur- Mass of packing 993 g
rent, countercurrent, and jacket cooling scarcely have been
reported in literature. Mass of shell 2020 g
The objective of the present study includes the evolution of
engineering definitions for bed operation and control along
with the determination of engineering bed configurations like
cocurrent, countercurrent, and jacket cooling. Bed switching
conditions were also determined. Minimization of energy and
maximization of separation was explored. The concepts of flow
variations and operational stability of the cryogenic beds under
bed saturation conditions were studied. In a preliminary study,
experiments were conducted under atmospheric pressure and
both CO2/N2 and CH4/CO2 binary mixtures were used. Opti-
mal hybrid cryogenic separation networks for natural gas with
higher hydrocarbon mixtures at high pressures have been
reported by Maqsood et al. [10]. The energy requirement in
switched countercurrent cryogenic beds with efficient process
controls during bed switching is evaluated and compared with
the conventional cryogenic distillation process.

2 Desublimation-Based Switched
Countercurrent Cryogenic Separation
of CO2
The experimental setup consists of stainless-steel jacketed cryo-
genic beds packed with glass balls, a cooling system, and a gas
feeding system. The physical dimensions of the experimental
setup are provided in Tab. 1. Several thermocouples were used
to investigate the temperature changes within the bed. Provi-
sion was made for liquid nitrogen to be introduced either into
the inner shell or into the jacket. The gas feeding system com-
prised of a gas chamber with multiple inlets for mixing differ-
ent gases. There were two sampling devices attached to the set-
up and the samples were subsequently transferred to the
sampling bag for analysis using a GC unit (Shimadzu GC
2010). Auxiliary continuous measurement with an IR gas ana-
lyzer (MRU Vario Plus) was also undertaken. The experimental
setup for cryogenic separation of CO2 is illustrated in Fig. 1.
Under atmospheric pressure, CO2 and CH4 have freezing
points of –78.5 C and –182.5 C, respectively, and it is conven-
ient to separate the mixture of these components based on the
difference in freezing points. In cryogenic separation, CO2
desublimates on the surface of prechilled packing and CH4
passes without any phase change. The overall process involves
three different cycles, namely, cooling of the packing surface,
capture of CO2 gas, and subsequent recovery of CO2 gas. In the
CO2 capture cycle, a mixture of CO2 and CH4 of varying con-
centration is introduced in the packed bed, CO2 desublimates
Figure 1. Experimental setup for separation of CO2 using a
switched cryogenic packed bed.
on the surface of the packing, and CH4 passes through without
any phase change. When the bed was filled with frost layer of
CO2 or when a small quantity of CO2 was detected in the outlet
stream, the supply of feed was cut off and the recovery of CO2
was started. Three different initial bed temperature profiles
were selected for experiments: temperature profile 1 with –90,
–82, –73, –68 C, temperature profile 2 with –93, –85, –83,
–71 C, and temperature profile 3 with –103, –97, –89, –83 C.
Since inferential advanced control was not applied in the pres-
ent study, the bed temperature profiles may have a load dis-
turbance up to maximum of ± 3 C.
The output gas samples were collected in sampling bags and
GC analysis was conducted along with continuous IR measure-
ments. The GC results were calibrated at 98 % CH4 and 2 %
CO2. An example of the calibrated GC result is presented in
Fig. 2.
In the recovery cycle, the frosted CO2 was recovered from
the system by raising the bed temperature above the freezing
point of CO2 by introduction of a CO2 stream at room temper-
ature. The complete process concept using two different beds is
illustrated in Fig. 3. When bed 1 reaches the saturation point,
the capture cycle is completed and the feed is switched to bed 2,

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 Research Article
Figure 2. Sample GC result for a mixture of 98 % methane and 2 % CO2.
which is at the desublimation point of CO2. Bed 1 is then
shifted to the CO2 recovery cycle. After completion of the
recovery cycle, it is again shifted to the cooling cycle. The
switching cycle of the two beds dictates the energy economy of
the process.
Figure 3. Schematic diagram of a switched countercurrent cryogenic packed bed.
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3 Effect of Flow
Configuration
on Cryogenic Separation
Two ways are possible to introduce the feed
into the switched cryogenic packed bed,
namely cocurrent and countercurrent, with
reference to the direct introduction of liq-
uid nitrogen. Presently available literature
[5, 6] considers the entire bed at constant
or average temperature. However, mainte-
nance of entire beds at constant tempera-
ture was found to be almost twice or more
energy-intensive compared to the distribut-
ed temperature in separation beds. It was
observed that CO2 feed at 20 C causes the
inlet side temperature to change rapidly
and, therefore, the experimental dynamics
of bed temperature profile and subsequently
separation performance of switched cryo-
genic packed beds differ considerably based
on flow configuration of feed CO2 and liq-
uid nitrogen or coolant.
3.1 Countercurrent Flow Configuration
The schematic diagram for the countercurrent flow arrange-
ment is presented in Fig. 4 a. The inlet direction of liquid nitro-
gen at z = 1 is countercurrent to the direction of CO2 inlet at
z = 0. The initial bed temperature profile is measured to be
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1678 Research Article

–97, –90, –85, –82 C in the direction of

liquid nitrogen flow. The feed flow rate of
100 % CO2 is controlled at 5 L min–1.
The experimental results for countercur-
rent feed flow are indicated in Figs. 5 a and
b. The change in concentration along with
the rise in bed temperatures at different
locations are measured by T1, T2, T3, and
T4. It is elucidated from Fig. 5 b that T4 pre-
sented a sharp rise in bed temperature
immediately after start of the capture cycle
at 6 s because of the entry of warm CO2 gas
at 20 C. Also CO2 converts from gaseous
feed into a solid phase upon entry and then
the solid CO2-forming layer moves towards
the colder end of the bed. According to
Fig. 5 b, the temperature at the exit end, T1,
remains at –90 C up to about 190 s. Hence,
maximum CO2 deposition occurs at the
Figure 4. Schematic diagram of a single cryogenic packed bed with (a) countercurrent exit end and may lead to operational block-
and (b) cocurrent flow configuration. age under certain conditions. This phe-
nomenon has been termed as operational

a) c)

b) d)

Figure 5. Experimental measurement of CO2 concentration and bed temperatures in the cryogenic packed bed with countercurrent
(a, b) and cocurrent (c, d) flow configuration.

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 Research Article 1679

saturation. After considerable time in the capture cycle, the Table 2. Energy comparison between cocurrent and counter-
CO2 gas finds a passage through the solid phase. The time and current flow.
conditions at which the first change of CO2 concentration is
observed at the exit, i.e., at z = 1, is termed in this study as bed Mode of feed flow
saturation which is illustrated in Fig. 5 a. Countercurrent Cocurrent
After 198 s, the bed is at the saturation point, which means
that no more CO2 can be captured and at this time the outlet Saturation time [s] 195–200 140–145
CO2 concentration is approximately zero. Once the bed is satu- Mass accumulated [kg] 0.0323 0.0228
rated (198 s in Fig. 5 b), the outlet CO2 concentration increases
since no further desublimation of CO2 occurs. The outlet con- Total heat duty [kJ] 22.95 17.55
centration of CO2 finally reaches the feed composition. This 1 ]
Q [kJ kgCO 680–710 750–768
2
time is termed as bed critical point. It approximately took 40 s
(Fig. 5 a) to reach 100 % CO2 concentration, which is the bed
critical point. The cryogenic bed ceases to function at the bed current flow configuration with higher energy efficiency will be
critical point. Fig. 5 b indicates that the bed temperatures T4, subsequently studied in the present work.
T3, T2, and T1 rise above the freezing temperature after 6, 76,
98, and 198 s, respectively, under the bed operating conditions.
The cryogenic bed is switched to the recovery cycle at the bed 4 Effects of Feed Flow Rate,
saturation point to recover the deposited CO2 and minimize Bed Temperature Profile, Feed
the energy requirement. In industrial applications with contin- Composition, and Bed Pressure
uous feeding of pipeline gas into the cryogenic bed, the failure
of switching operation causes CO2 to get mixed with the sepa-
on Cryogenic Separation
rated methane. This may reduce both the separation and ener-
The influence of feed flow rate, feed concentration, and initial
gy efficiencies of the process. Advanced inferential controller
bed temperature profile on cryogenic bed saturation was deter-
development for this application will be reported in future pub-
mined. Different ranges of feed flow rate (2, 5, and 10 L min–1)
lications.
were employed for the experimental study at the three selected
bed temperature profiles. The feed composition was varied
from 13 % to 100 % CO2.
3.2 Cocurrent Flow Configuration
The results presented in Fig. 6 a with feed gas CO2 composi-
tion of 100 % at 2, 5, and 10 L min–1 and initial bed temperature
The schematic diagram for the cocurrent feed flow is presented
profile of –90, –82, –73, –68 C demonstrate a considerable
in Fig. 4 b. The entry direction for both feed and refrigerant is
change in saturation time, namely 220, 55, and 36 s, respective-
similar at z = 1 though the two flows are separated in time
ly. The results for feed gas with CO2 composition of 40 % at
cycles. The experimental result for cocurrent feed flow are dis-
–98, –94, –83, –71 C are presented in Fig. 6 b.
played in Figs. 5 c and d. The initial bed temperature profile at
Simulation results were compared with experimental meas-
the end of the cooling cycle was measured to be –97, –90, –85,
urements in Fig. 6 a. A cryogenic packed bed has been modeled
–82 C. A feed containing 100 % CO2 at 5 L min–1 was used in
in literature using the following equations [5, 7, 12]:
this experiment.
In cocurrent flow configuration, the temperature of the cryo-  
genic bed at the feed entry point is the minimum, namely ¶C ¶C ¶ ¶C
erg þ rg vg ¼ rg Deff þS (1)
–97 C, due to the warm CO2 entry and solidification of the ¶t ¶z ¶z ¶z
feed, the rise in inlet bed temperature T1 is very sharp, and in
46 s the desublimation temperature of CO2 was crossed. ¶T ¶T
The temperature profile of the other exit end of the bed, T4, ðerg cp;g þ rs ð1  eÞcp;s Þ þ erg vg cp;g
¶t ¶z
also increased above the freezing temperature within 73 s.
Therefore, the deposition mainly remained constrained in the ¶ ¶T
¼ ðl Þ þ Sh (2)
middle section of the bed as shown by the crossover times of ¶z eff ¶z
140 and 147 s for T2 and T3, respectively. Therefore, it can be
inferred that in the case of cocurrent flow configuration, less The symbols are explained in the list at the end of the paper.
availability of the bed for desublimation caused a large reduc- The effect of the initial cryogenic temperature of a packed bed
tion in bed saturation and the CO2 deposited. The energy com- on bed saturation is indicated in Fig. 6 c for a feed flow rate of
parison between countercurrent and cocurrent flow configura- 5 L min–1 with 100 % CO2. The bed saturation point is directly
tions is provided in Tab. 2. It can be observed that the energy dependent on the cooling energy used within the packed bed.
requirements for countercurrent are less than the cocurrent A lower initial bed temperature profile generates higher satura-
flow configuration. tion time. It can also be concluded that for the higher composi-
The cocurrent flow configuration displays higher probability tion of CO2 in the feed, the amount of CO2 capture became
for the operational saturation because of sublimation and rede- higher.
position of CO2 at the center of the cryogenic bed with temper- Fig. 6 d illustrates the effect of CO2 feed concentration
ature rises at both ends. Based on these observations, counter- change from 13 to 100 % at fixed flow of 5 L min–1 on bed satu-

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1680 Research Article

a) b)

c) d)

Figure 6. Effect of (a, b) flow rates, (c) initial bed temperature, and (d) feed composition on bed saturation time.

ration time with bed temperatures of –104, –101, –94, –83 C. 5 Effect of Feed Flow Rate,
It is evident that the higher CO2 concentration in the feed Bed Temperature Profile, and Feed
increases the bed saturation from 60 s for 13 % CO2 to 260 s for
100 % CO2. This is due to the fact that a lower CO2 concentra-
Composition on the Energy
tion in the feed further decreases the desublimation tempera- Requirement in Switched Cryogenic
ture of CO2. Packed Beds
A case study to investigate the effect of jacket cooling and
direct cooling on saturation time is illustrated in Fig. 7 a. Tem- The influence of feed flow rate, bed temperature profile, and
perature profile 2 with 5 L min–1 feed flow rate was employed. feed composition on the energy requirement of the switched
As expected, the jacket cooling configuration exhibited a longer cryogenic packed bed was studied. The required energy in the
bed saturation time as compared to direct cooling. In order to cooling cycle can be calculated as:
conduct experiments at higher pressure, the cryogenic bed was Z Tf
first pressurized with feed gas and jacket cooling was per- Q¼ ðmp cp p þ msh cp sh Þ dT (3)
formed. Fig. 7 b illustrates the effect of bed pressure on satura- Ti
tion time. It is evident that a higher bed pressure substantially
decreases bed saturation time. The energy transfer during capture cycle can be determined
as follows:
QC ¼ ðmCO2 cpCO2 DT þ mCO2 lCO2 Þ þ QSur (4)

An example of the energy cycles based on the experimental

setup reported in this paper is presented in Fig. 8.

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 Research Article
a)
b)
Figure 7. (a) Effect of jacket cooling and direct cooling and (b) effect of pressure on bed
saturation time.
Based on saturation times reported in Fig. 6 a, the mass accu-
mulated and energy requirements are presented in Tab. 3. The
energy requirements for the flow rate of 2, 5, and 10 L min–1
were 795, 635, and 621 kJ kg1
CO2 (Fig. 9). The saturation time
for lower flow rates is higher and the heat leakages were also
comparatively higher as elucidated in Tab. 3. The effect of 40 %
CO2 composition in the feed on the energy is given in Tab. 4.
The influence of the initial bed temperature profile on the
energy requirement is indicated in Tab. 5. Three different initial
bed temperatures were selected (Fig. 6 c). The feed flow rate of
5 L min–1 and feed CO2 composition of 100 % were kept con-
Chem. Eng. Technol. 2014, 37, No. 10, 1675–1685 ª 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
1681
stant. The lower bed temperatures resulted
in longer bed saturation times with in-
creased amount of deposited CO2. In case of
bed temperature profile 1 with higher tem-
peratures (–89.7, –82.1, –72.7, –67.9 C), the
saturation time is 60 s and the deposited
amount is 0.00979 kg. The energy require-
ment was found to be 635 kJ kg1 CO2 . A bed
saturation time of 235 s and 0.0383 kg of
CO2 deposited was observed for bed temper-
ature profile 3 (–103, –97, –89, –83 C). This
corresponds to 726 kJ kg1 CO2 energy require-
ment. It is evident from Tab. 5 that by de-
creasing the bed temperature, the energy re-
quirement and amount of CO2 deposited
also increases. The higher energy require-
ment for low bed temperature profiles were
caused by the cooling loads and the increase
in heat leakages from the surrounding due to
the longer saturation time.
The composition of feed has a significant
effect on the energy demand during the
cryogenic capture cycle as observed in
Fig. 6 d. For the same flow rate and initial
bed temperature, the saturation time be-
comes longer with increase in feed compo-
sition. The influence of feed composition
on energy is illustrated in Fig. 9. The energy
requirement for low composition of CO2 is
greater as compared to the higher composi-
tion of CO2, i.e., for 13 % CO2 in feed it is
1857 kJ and in the case of 100 % CO2 it is
747 kJ. The energy requirements for differ-
ent feed composition of CO2 are given in
Tab. 6.
The energy requirements for both jacket
cooling and direct cooling were calculated
from data available in Fig. 7 a. The satura-
tion times for jacket cooling and direct
cooling are approximately 180 and 150 s,
respectively. The energy requirements for
jacket cooling and direct cooling are about
900 and 700 kJ kg1CO2 , respectively.
6 Comparison of Energy Requirements
of a Desublimation-Based Packed Bed
and Conventional Cryogenic
Distillation
Ryan and Holmes [11] developed an extractive cryogenic distil-
lation network by adding n-butane in the condenser of the dis-
tillation column to avoid CO2 solidification. A ready-to-trans-
port liquid CO2 product flow can be obtained in cryogenic
distillation. A comparative study between energy requirements
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1682 Research Article

Figure 8. Energy change during cooling, capture, and recovery cycles in a switched cryogenic bed.

Table 3. Effect of flow rate on energy requirement. Table 5. Effect of initial bed temperature on energy require-
ment.
Feed flow rate [L min–1]
Initial bed temperature
2 5 10
Temperature Temperature Temperature
Saturation time [s] 210–220 55–60 35–40 profile 1 profile 2 profile 3
Mass accumulated [kg] 0.01423 0.00979 0.01171 Saturation time [s] 60 150 235
Total heat duty [kJ] 11.32 6.22 7.28 Mass accumulated [kg] 0.00979 0.02450 0.03830
1 ]
Q [kJ kgCO 795 635 621
2 Total heat duty [kJ] 6.22 16.38 27.83
1 ]
Q [kJ kgCO 635 669 726
2

Table 4. Effect of flow rate on energy requirements for 40 %

CO2 concentration in the feed.
tion columns was 0.00086 kg s–1. Condenser and reboiler duties
Feed flow rate [L min–1] for this mass removal were calculated as 1.2662 kJ s–1. The energy
required per kg of CO2 was found to be 1472 kJ kg1 CO2 .
15 5 According to Fig. 9 the total energy required for the cryogen-
Saturation time [s] 20–30 55–60 ic packed bed was 765 kJ kg1 CO2 . Interestingly, for the higher
CO2 contents in natural gas the cryogenic packed bed provides
Mass accumulated [kg] 0.01225 0.00976 a promising potential for industrial exploitation.
Total heat duty [kJ] 10.69 9.52
1 ]
Q [kJ kgCO2
873 975 7 Conclusions
The present study attempts to bridge the gap in existing litera-
in a conventional cryogenic distillation network (Fig. 10) and ture through a systematic study of engineering parameters like
switched cryogenic packed bed is presented. flow configurations, flow rates, bed temperature distribution,
A feed with 30 % CH4 and 70 % CO2 was selected with a flow and bed saturation times during purification of natural gas
rate of 100 mol h–1. Mass flow rates in all columns are given in with high CO2 content. The switching cycles were obtained for
Tabs. 7 and 8. The energy required per kg of CO2 was calculated best energy utilization. The performance of the switched coun-
based on these mass flows. The net CO2 removal in the distilla- tercurrent cryogenic bed was substantially superior to other

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 Research Article 1683

Figure 9. Effect of feed composition and flow rate on the energy requirement.

Figure 10. Scheme of cryogenic distillation for removal of CO2 from natural gas.

flow configurations. A detailed experimental study for both Acknowledgment

mass and energy transfer was performed. The energy consump-
tion of switched countercurrent operations is compared with The authors gratefully acknowledge the financial and infra-
the conventional cryogenic distillation process. The energy re- structural help from YUTP project and Department of Chemi-
quired for conventional distillation was 1472 kJ kg1
CO2 as com- cal Engineering, Universiti Teknologi PETRONAS.
pared to the cryogenic packed bed energy requirement of
810 kJ kg1
CO2 for the same feed composition. The effect of feed The authors have declared no conflict of interest.
composition on the energy requirement revealed that counter-
current switched cryogenic packed beds have potential for sub-
stantial energy savings during purification of natural gas with
high CO2 content.

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1684 Research Article

Table 6. Effect of feed composition on energy requirement (bed temperatures: –104, –101, –94, –83 C)

CO2 in feed [vol %] Saturation time [s] Mass accumulated [kg] Total heat duty [kJ] 1 ]
Q [kJ kgCO2

13.00 60 0.00171 3.70 1857.43

46.00 80 0.00673 7.02 1043.74

61.00 130 0.01677 14.18 845.31

76.00 200 0.02731 21.79 798.03

100.00 260 0.04247 31.75 747.61

Table 7. Net CO2 removal in distillation columns.

Column 1 Column 2 Column 3 Column 4

No. of stages 10 12 10 20

CO2 in [kg s–1] 0.00086 0.00037 0.00012 0.00006

CO2 out [kg s–1] 0.00037 0.00012 0.00006 0.00000006

Butane [mol h–1] 0 10 10 10

Table 8. Flow rate and energy requirement in distillation columns.

Feed (mole fraction) Flow rate [mol h–1] Distillate (mole fraction) Flow rate [mol h–1]

CH4 CO2 Butane CH4 CO2 Butane

Column 1 0.30 0.70 0.00 100 0.4999 0.5001 0 60

Column 2 0.4285 0.4286 0.1429 70 0.7498 0.2448 0.0053 40

Column 3 0.6024 0.1967 0.2009 49.79 0.8568 0.1403 0.0029 35

Column 4 0.6679 0.1093 0.2227 44.90 0.9985 0.0001 0.0013 29.5

–1 1 ]
Bottom (mole fraction) Flow rate [mol h ] Energy [kJ kgCO2

CH4 CO2 Butane Condenser Reboiler Total

Column 1 0.0001 0.9999 0 40 650 322 0.16

Column 2 0.0001 0.6737 0.3262 30 716 563 0.14

Column 3 0.0003 0.3256 0.6741 15 2507 2646 0.16

Column 4 0.0343 0.3165 0.6493 15.5 1416 1372 0.08

a)
in [mol h–1].

Symbols used T [K] temperature

v [m s–1] superficial velocity
as [m2m–3] specific surface area z [m] axial position
C [–] concentration v/v
cp [J kg–1K–1] heat capacity
Deff [m2s–1] effective diffusion coefficient
Greek letters
h [J kg–1] enthalpy
m [kg] mass l [J m–1K–1s–1] thermal conductivity
Q [kJ] heat duty leff [J m–1K–1s–1] effective thermal conductivity
S [kg m–3s–1] source term r [kg m–3] density
t [s] time e [–] porosity

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 Research Article 1685

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