Process Simulation Research of CH4/N2 Separation

Gaobo Zhang, Shuanshi Fan, Xuemei Lang, Yanhong Wang*

The Key Laboratory of Enhanced Heat transfer and Energy Conversation,
Ministry of Education, South China University of TechnologyGuangzhou, China,
*Corresponding authare-mail: wyh@scut.edu.cn

AbstractThe separation energy consumption of methane and

nitrogen mixture of 3 kinds of typical method, Cryogenic (DC),
Pressure Swing Absorption (PSA) and Membrane (MEM), was
calculated by Aspen Plus in this paper. The result shows that
at 35, the ratio of methane and nitrogen is 1, the separation
energy consumption of 3 methods are 5.2, 3.6 and
2.6104kJ/kmol, respectively. The ratio of calculated energy
consumption to theoretical consumption is 2.3, 1.6 and 1.2, the
energy consumption of DC is the highest, then PSA, MEM is
lowest. This work is to give some reference for the selection of
CH4/N2 separation.

Keywords- CH4/N2; Gas Separation; Energy Consumption;

Process Simulation

C2
Cooler

HE#2
J1
Heat Exchanger Depressure Valve
13

15

14

12

11

CP2
Compressor
10

Off gas

Raw gas

4
19

20

LNG

18

CP1
Compressor

17

16

C1
Cooler

C3
HE#1
Cooler Heat Exchanger

J1
HE#3
CP3
EP1
Compressor Expander Heat Exchanger Depressure Valve

T1
Separator

Fig.1 CH4/N2 cryogenic process

II.

1 CH4/N2 SEPARATION FLOW SIMULATION AND

ENERGY CONSUMPTION ANALYSIS

A. 1.1 Cryogenic
I.

INTRODUCTION

Natural gas(NG), coal bed methane(CBM) and oil field

associated Gas(OFAG) etc. are the important energy source,
which main components are methane and some unavailable
gases such as N2, CO2 and H2S, etc. These impurities restrict
the usage and reduce their value. For example N2 in NG and
CBM will lower the heat enthalpy and lead to these gases
cannot use for fuel of motor or some chemical raw material.
By common gas separation methods, it is easier to take out
some polar compounds like CO2 and H2S, but it is difficult to
separate N2 from CH4. So the separation process for the N2
and CH4 has become the hot research spot in the world.
At present, the common methods for the N2 and CH4
separation are Cryogenic (CRG), Pressure Swing
Absorption(PSA) and Membrane(MEM). Some researches
[1-10] have given amount of process simulation and
optimization results, but there is few analysis and
comparison of separation energy consumption, so it is
difficult to optimize and combine these 3 methods for energy
conservation.
The separation energy consumptions of DC, PSA and
MEM are calculated and analyzed for the mixed gas by
Aspen Plus simulation software in this paper. Compared with
the mixed gass theoretic separation consumption, the energy
consumption rank is given, which is the foundation for
selecting the best process route in energy consumption.

B. (1) Process Flow Design

This paper selects the flow of nitrogen expanding &
liquefaction with C3H8 pre-cooling. The process is simple
and compact and we can lower the energy consumption
effectively by using this high efficiency way in high
temperature zone by introducing the C3H8 pre-cooling. The
flow diagram shows in Fig.1 The raw material CH4/N2
mixed gas is firstly compressed, cooled through the
Circulating Water(CW) cooler, C3H8 pre-cooling and N2
cooling; then lowered its pressure by the pressure reducing
valve; finally separated the product LNG from the vaporliquid separator. The tail gas goes through the HIM #3 and
HIM #1 to recovery the cooling quantity. Propane precooling is a vapor compressing cool-making circulation.
During the nitrogen expanding circulation, nitrogen is precooled in HE#1 by compressed and CW cooled, then
producing cooling in expander to supply HE#3.
C. (2) Process simulation and energy consumption
analysis
Simulate the process by Aspen Plus with the base data
from Tab.1.
The energy consumption of cryogenic method includes
that from feed compressor, propane pre-cooling compressor,
nitrogen cool-making compressor, expander and coolers. By
the simulation and analysis, we can get the liquefied ratio,
methane recovery ratio, purity and separation energy
consumption of unit liquefied product corresponding the
different raw gas composing. Conclusion from Fig.2, along

TABLE I.

CRYOGENIC SIMULATION CONDITION

Item

Off gas

Simulation Parameters
4 5

Raw gas
C3H8 precooling
N2
cooling
Off gas

P1=0.1MPa,T1=35,P2=1MPa,T3=35,T4=-35,T5=145,P6=0.2MPa
P12=2MPa,T13=35,T14=30,T15=-33

12

P17=1MPa,T18=35,T19=-35,P20=0.2MPa,T16=-20

Product gas

P10=30

Product

P7=0.2MPa

Compress
or
Expander

e=0.75,m=0.95

Cooler

Pressure drop=0

Raw gas
1

e=0.75,m=0.95

recovery

0.4

30000
20000
10000
0

liquefying
rate

0.2
0

0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9

methane mol%
Fig.2

Energy consumption
kJ/kmol

purity/recovery
/liquefying rate

energy
consumption

0.8
0.6

70000
60000
50000
40000

purity

E.

Energy consumption corresponding to different CH4 composition

with DC process

1.2 PSA

(1) Process Flow Design

PSA process selected has a 3 column continuing
operation, including 5 steps, absorption, current pressure
reducing, countercurrent pressure reducing, vacuum and
pressure building (As showed in Fig. 3).
Absorption Step (AS): the CH4/N2 gas is mixed,
compressed and cooled then goes through the absorption bed
from its bottom. The easier absorbed compounds (CH4) are
enriched, and more difficult ones (N2) flow out of the bed.
Along with the direction of absorption bed, the absorption
wave forms and the step stop when the wave transfers to the
bed.
Current Pressure Reducing Step (CPR): cutting the gas
flow, pressure reducing the absorption bed till the absorption

T1/2/3
Adsorption Tower

10

11

V1
CP3 CP2
CL2
Vacuum vessel Pump Compressor Cooler

Fig.3 PSA flow diagram for CH4/N2

TABLE II.
Item
Raw gas

PSA SIMULATION CONDITION

Simulation Parameters

P1=0.1MPa,T1=35,P2=1MPa,T3=35

Adsorbent bed

Absorbent type:T103 active carbon[11], Saturation

adsorb amount of CH4 and N2 are 110.3ml/g and
68.7ml/g respectively, Separation factor of CH4/N2 is
2.9,Langmuir adsorption equilibrium constant of CH4
and N2 are 1.034 and 0.572,Absorbent amount is
0.82kg
Height=0.1m,Diameter=0.04m,Void rate=0.395

User-defined
PSA model

Tpes+Tas=180s,
TCPR=60s,TcCPR+TVs180s,Pas=1MPa,PCPR=0.2MPa,PcCP
R=0.1MPa,Pvs=0.05MPa

Compressor

e=0.75,m=0.95

Cooler

Pressure drop=0

with the increase of methane concentration in raw gas,

the one in product gas increases, simultaneity the decrease of
methane recovery ratio, liquefied ratio and separation energy
consumption.
D.

3
6

CP1
CL1
Compressor Cooler

1.2

V2
Product vessel

Adsorbent

wave arrives at the discharge as the symbol of this step

finishing.
Countercurrent Pressure Reducing Step (CCPR): along
with the pressure reducing, the methane gas absorbed as
product is released from the sorbent and comes out from the
vessel. Stopping the step till the pressure goes down to a
defined point.
Vacuum Step (VS): Putting a vacuum pump to suck
out the residual gas to make the sorbent regenerated.
Pressure Building Step(PBS): Resume the pressure by
filling of the gas.
F. (2) Process simulation and energy consumption
analysis
As a dynamic process, for simulation by using ASPEN
PLUS, the PSA is processed as a whole steady unit by
calculating the average flowrate of the feed gas from the step

35000
30000

0.8

25000

0.6

20000
energy
consumption

recovery
0.4

15000
10000

0.2

5000

0
0.4

Product purity and recovery

rate

0.9

Fig.4

0.6
0.7
0.8
raw gas methane mol%

0.9

21700
purity

0.7
0.6

21650
21600

recovery

21550

0.5

21500

0.4

energy
consumption

0.3

21450
21400

0.2

21350

0.1

21300

0
0.5

21750

0.8

21250
0.4

Energy consumption corresponding to different CH4

composition with PSA process

of pressure building and absorption as the feed gas, of the

discharge gas from the step of absorption and current
pressure reducing as the discharge gas, of the desorption gas
from the step of count-current and vacuum as the product gas.
For no existing PSA model in ASPEN PLUS, a external
Excel subprogram is creativity used to calculate the tail gas
flowrate and composition. Base date sees Tab.2
Energy consumption in PSA unit mainly comes from
feedstock compressor, product vacuum pump, product
compressor and coolers. Fig.3 shows the relation between
the feed gas composition and the energy consumption of unit
product.
From Fig.4, we can see the higher of the methane
concentration in feed gas, the higher of the one in product
gas, the lower of the energy consumption for the unit product
gas and the lower of the methane recovery ratio.
G. 1.3 Membrane Process Simulation and Analysis
H. (1) Process Flow Design
The model of hollow fiber membrane separator is
selected for CH4/N2 in this paper. The model assumes 4
aspects, the dominant flow direction is contrary with its
infiltration flow direction, no pressure drop between feed
side and infiltration side, the infiltrativity of member
independent with the pressure and concentration, and ignores
Off gas

Infiltration gas

Fig.6

0.5
0.6
raw gas methane mol%

0.7

0.8

Energy consumption corresponding to different CH4 composition

with membrane process

the effect of support layer. Fig 5 shows the process flow. The
CH4/H2 mixing gas is compressed and cooled before to a
buffer vessel then to the membrane unit. For the infiltration
ratio of methane is bigger than nitrogen, the rich methane gas
across from the membrane to another buffer vessel, then to
product vessel after compressed and cooled. The tail
infiltration gas rich nitrogen comes out from the other side of
the membrane.
I.

(2) Process simulation and energy consumption

analysis
A user-defined separation model is built in ASPEN
PLUS by calling the external Excel subprogram to calculate
the composition of infiltration gas and tail gas.
Energy consumption in membrane unit mainly comes
from feedstock compressor, product compressor and coolers.
Fig.6 shows the relation between the feed gas composition
and the energy consumption of unit product.
From Fig.6, we can see the same rule with PSA, that the
higher of the methane concentration in feed gas, the higher
of the one in product gas, the lower of the energy
consumption for the unit product gas and the lower of the
methane recovery ratio.
III.

2 THREE SEPARATION PROCESSES ENERGY ANALYSIS

AND COMPARISON

A. 2.1 Theoretical Separation Energy Calculation

Raw gas
6

CP1
CL1
Compressor Cooler

Fig.5

D1
Buffer vessel

M1
Membrane unit

D2
CL2
D3
CP2
Buffer vessel Compressor Cooler Product vessel

Membrane flow diagram for CH4/N2

B. (1) Minimum Gas Separation Energy consumption

Calculation
theorical separation energy
consumption,kJ/kmol

Energy consumption,kJ/kmol

40000
purity

Energy consumption,kJ/kmol

Product purity and

recovery rate

1.2

Fig.7

24000
23500

energy
consumption

23000
22500
22000
21500
0

0.2

0.4
0.6
0.8
1
raw gas methane mol%
Min GSE corresponding to different CH4 composition

TABLE III.

MEMBRANE SEPARATION SIMULATION CONDITION

Item

Simulation Parameters

Raw gas

P1=0.1MPa,T1=35,P2=1MPa,T3=35

User-defined
separation model

Compressor

Membrane type: PDMS, Permeability of CH4 and

N2 are 110-10kmol/(m2sPa) and 3.361011
kmol/(m2sPa) respectively, separation factor
of CH4 is 3
e=0.75,m=0.95

Cooler

Pressure drop=0

The Minimum Gas Separation Energy (Min GSE) is the

minimum energy consumption of the mixed gas separation
process and can be calculated with exergy formula. Flowrate
N in mol/h, the composition of product methane and product
nitrogen is y1 and y2 in mol% and in the same pressure P0
and temperature T0. Subscript a for product methane and b
for product nitrogen. The method for the Min GSE
calculation shows below:
Calculate the exergy under the purity material and in
the standard situation P0 and T0.
Exergy of unit mol feed gas:
Exf=HfH0T0SfS0
Of which
HfH1y1H2y2 H
H0=H1y1H2y2

Sf=S1y1S2y2Ry1lny1y2lny2 SE
(4)
TABLE IV.
Separation
process

S0=S1y1S2y2

Based raw gas and products for the ideal mixture, that
is, H=0, SE=0, so raw gas exergy:
Exf=RT0y1lny1y2lny2
(6)
Product exergy:
Ex1=RT0ya1ln ya1ya2ln ya2
(7)
Ex2=RT0yb1ln yb1yb2ln yb2
(8)
Therefore the required minimum energy of feed gas ( N
mol/h) separated into two flows (Na and Nb mol/h) at
pressure P0 and temperature T0 is:
Wmin= Ex=NaEx1NbEx2NExf
(9)
C. 2Theoretic Separation Energy Consumption
Analysis
The gas theoretic separation energy consumption
includes the feed gas energy consumption of compression,
cooling energy consumption and minimum separation of
power. Through simulation analysis, with certain product
concentration and recovery of methane gas, the theoretic
separation energy consumption of different composed
materials can be obtained. Figure 7 shows the theoretic
separation energy consumption of the different feed gas
concentrations of methane at the 10bar, 35 . The
methanegas concentration is 0.9 and recovery is 0.9. Seen
from Figure 7, gas theoretic separation energy consumption
decreases with the increasing of methane concentration of
feed gas.

CH4/N2 SEPARATION PROCESS ENERGY CONSUMPTION

CH4
Recovery

CH4
Purity

Energy
consumption,
104kJ/kmol

Ratio to
theoretical
energy
consumption

Min GSE model

0.9

0.9

2.3

DC

0.91

0.63

5.2

2.3

PSA

0.75

0.89

3.6

1.6

Membrane

0.64

0.72

2.7

1.2

Energy Consumption
composition

Influencing factors

Power consumption of
compressor; Cooling energy
consumption,
min GSE
Power
consumption
of
compressor; Cooling energy
consumption,
both raw and product
Power
consumption
of
compressor; Cooling energy
consumption,
both raw and product
Power
consumption
of
compressor, Cooling energy
consumption,
both raw and product

Composition,
pressure
and
temperature of raw gas, CH4
recovery and purity of product
gas.
Composition,
pressure
and
temperature of raw gas;
Flowrate,
pressure
and
temperature of refrigerant.
Composition,
pressure
and
temperature of raw gas;
Adsorbent parameters;
PSA cycle parameters
Composition,
pressure
and
temperature of raw gas;
Membrane and relevant device
parameters;

D. 2.2 Separation Technology Analysis and Comparison

of Energy Consumption
At 10bar, 35, the molar composition of methane and
nitrogen both were 0.5 feed gas was separated into two
gas products. Under the simulation condition of Table 1,
Table 2 and Table 3, it get the products recovery,
concentration and energy consumption data of three
processes through DC separation, PSA and membrane
separation process simulation technology (detail see Tab.4).
(1) Table 4 shows that the energy consumption of three
kinds of separation technology are all from the compressor
and cooling energy consumption, and they are comparable.
In the same feed gas and the separation conditions, the DC
separation process has the maximum energy consumption,
PSA followed, membrane separation minimum, but all are
greater than the theoretic separation power, and this is also
consistent with the reference about the energy consumption
of qualitative comparison of three processes [12].
(2) From Figure 2, Figure 4 and Figure 6, to a certain
pressure and temperature, and the selected separation
conditions, the feed gas composition is the most important
factors for the energy consumption. Methane concentration
of feed gas increased separation energy consumption
reduced. Besides the feed gas composition, the influence
factors of separation process for the specific energy
consumption are not the same. The energy consumption of
DC separation process is related with refrigerant parameters,
PSA process with adsorbent parameters, and membrane
separation technology closely with the membrane
parameters.
(3) For the different feed gas composition, the suitable
separation process is different. See figure 2, figure 4 and
figure 6, for relatively low concentrations of methane feed
gas, DC separation process is better; for relatively high
concentrations, DC or membrane separation technology are
good; for relatively medium concentration, PSA method or
membrane, or combination of both process optimization are
proper. Optimization of separation processes will be the
main content of the follow-up study.
IV.

3 CONCLUSION

In this paper, Aspen Plus process simulation software is

used to build on CH4/N2 system three gas separation process
modeling. The PSA process is changed into a continuous
from batch operation by special method to meet the
requirements of the process simulation software.
Separation energy consumption of the three processes,
product purity and recovery ratio were calculated. The effect
the composition of feed gas on energy consumption of the
gas separation is analyzed. Meanwhile a preliminary
comparison is done for the separation process energy
consumption of three. The results show that the same feed
gas and the separation conditions, separation of cryogenic
technology most energy-intensive, PSA followed, membrane

separation minimum. The energy consumption is 2.3, 1.6

and 1.2 times of the theoretical separation energy
respectively.
Be noted that the separation energy analysis of the
three processes is on one simulation platform. It can not
fully explain the various processes of separation and energy
consumption. This is because besides raw materials,
separation energy also relate to the specific technology
process, separation of agent parameters and equipment
parameters, such as the cryogenic process, including cascade
refrigeration, mixing and expansion refrigeration cooling;
PSA has a variety of cyclic process; member separator
including hollow fiber membrane, flat plate and roll
separator. These specific processes and corresponding
equipment parameters will influence the process energy
consumption.
Next, we will select a combination of these three
processes to simulate, while using mathematical
programming method to search for different feed gas
separation technology, process optimization studies.
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