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Modeling Membrane Gas Separation in the Aspen Plus Environment

Article  in  Membranes and Membrane Technologies · August 2018

DOI: 10.1134/S2517751619010049

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ISSN 2517-7516, Membranes and Membrane Technologies, 2019, Vol. 1, No. 1, pp. 1–5. © Pleiades Publishing, Ltd., 2019.
Original Russian Text © A.A. Kozlova, M.M. Trubyanov, A.A. Atlaskin, N.R. Yanbikov, M.G. Shalygin, 2019, published in Membrany i Membrannye Tekhnologii, 2019, Vol. 9,
No. 1, pp. 3–8.

Modeling Membrane Gas Separation in the Aspen Plus Environment

A. A. Kozlovaa, b, *, M. M. Trubyanovb, A. A. Atlaskinb, N. R. Yanbikovb, and M. G. Shalygina
aTopchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences, Moscow, 119991 Russia
b
Department of Nanotechnology and Biotechnology, Nizhny Novgorod State Technical University,
Nizhny Novgorod, 603950 Russia
*e-mail: a_a_kozlova@ips.ac.ru
Received August 30, 2018

Abstract—The paper presents the results of the development of a unit for calculating mass transport in a mem-
brane gas separation apparatus in the Aspen Plus environment. The created user model has been verified by
comparing the results of the calculation of separation characteristics with available experimental data for two
cases. In the first case, the calculation results were compared with experimental data on the separation of the
ternary H2O/EtOH/N2 (13.3/5.5/81.2 mol %) vapor–gas mixture simulating the stream from the stripping
column of a laboratory membrane vapor separation unit with a plate-and-frame membrane module for eth-
anol recovery from fermentation broth. It has been shown that the calculated concentrations of the compo-
nents in the retentate and permeate streams are close to the experimental values obtained in the separation of
the ternary vapor–gas mixture. In the second case, the calculation results were compared with experimental
data obtained upon the separation of a binary N2/CH4 gas mixture (99/1 mol %) simulating a stream with a
low content of an easily penetrating impurity component using a disk-type membrane module. It has been
found that the calculated concentration of CH4 in the retentate is noticeably less than in the experiment,
especially at high stage cuts, a difference that is associated with the increasing influence of the longitudinal
diffusion of components at low speeds of the mixture in the channels of the membrane module, which dete-
riorates the separation characteristics of the apparatus with respect to the removal of impurities and requires
additional consideration of the deviation from the plug-flow mode in computational mathematical models
used for this case.

Keywords: membrane gas and vapor separation, mathematical modeling of membrane processes, Aspen Plus
DOI: 10.1134/S2517751619010049

INTRODUCTION the absence of phase transitions, and the hardware

Mathematical modeling is a powerful tool in the
development, study, and optimization of real techno-
logical processes. There are a large number of available
software products for the simulation of technological
processes that make it possible to build and explore
various process flow diagrams. Today, the Aspen Plus
software (developed by AspenTech©) is a leader in the
field of modeling technological processes of various
industries.
Currently observed tightening of requirements for
the quality of substances produced by the chemical
industry creates a trend towards the development of
new technologies and the optimization of existing
technologies [1]. In the field of gas separation, espe-
cially in the production of high-purity gases, a tech-
nology based on membrane gas separation can be con-
sidered as an attractive alternative to conventional,
energy-intensive processes [2]. The separation of gas
mixtures with the use of membranes is provided by the
physicochemical properties of the material, the pro-
cess conditions, and the technological parameters.
This process can be carried out at room temperature in
design is characterized by simplicity and easy scalabil-
ity. A variety of studies devoted to the development of
new materials and processes have been reported,
which show the promise held by this approach to solu-
tion of the problems of natural gas purification [3],
ammonia recovery [4], and deep gas purification [5]
and to invention of new nonstationary membrane sep-
aration processes [6]. In recent years, membranes have
also been used in the developing area of recovery of
bioalcohols (bioethanol, biobutanol). The energy-
saving membrane vapor separation method provides
concentration of bioalcohols to a high level from dilute
aqueous alcohol solutions formed in the fermentation
process [7]. In this regard, the implementation of a
multiparameter mathematical model that takes into
account the engineering and physicochemical aspects
of the process is an important task.
To fulfill the task, the Aspen Plus software package
was chosen, which has broad functionality and is
capable to simulate various chemical engineering
schemes and complex technological processes, as well
as to calculate energy costs and carry out economic

1
 2 KOZLOVA et al.

Feed JF
JR
stream cFi J(x) ci(x) J(x + Δ x) cRi Retentate
p
Δx
Membrane
0 x
M
L
J (x) p'
JP J '(x) c'(x) J '(x + Δ x)
Permeate i
cPi

1 Fig. 1. Schematic of mass transport in a membrane module for the countercurrent mode.

calculations. Aspen Plus contains a voluminous data- —change in a component flux upstream of the
base of physicochemical properties and thermody- membrane:
namic models, which allow prediction of properties
J i ( x + Δx ) = J i ( x ) − J i ( x ),
M
for both gaseous mixtures and liquids. With the use of (1)
the latest versions of Aspen Plus, it is possible to inte- —change in a component flux downstream the
grate design schemes created by the user in Excel [8], membrane:
thereby greatly expanding the possibilities of modeling
J i'( x + Δx ) = J i'( x ) − J i ( x ),
M
nonstandard blocks of the process scheme. Also, cus- (2)
tom models made in other software products can be
integrated into Aspen Plus. There are examples in the —component flux through the membrane:
literature of using the software platforms MATLAB J i ( x) = Qi B Δx Δpi ( x ),
M
(3)
[9] and FORTRAN [10] to create a custom model with
its subsequent export to Aspen Plus. —driving force for the transport of a component
Currently, Aspen Plus does not contain a ready across the membrane:
solution for modeling mass transport processes in Δpi ( x) = pci ( x ) − p'ci'( x ), (4)
membrane gas separation devices; however, the soft-
ware company (AspenTech©) provides, among other —mole fraction of the component upstream of the
things, the Aspen Custom Modeler (ACM) modeling membrane:
tool that focused on creating mathematical models of J i ( x)
ci ( x) = , (5)

its own, which can be used to design a custom mem-
brane block. The advantage of the model created in J i ( x)
i
ACM is the ease of exporting and binding it to Aspen
Plus, after which it can be used in the same way as —mole fraction of the component downstream of
other models already available in the Aspen Plus the membrane:
library.
J i'( x)
In this study, a gas separation membrane module ci'( x) = , (6)
was created in the ACM program and exported to
Aspen Plus for further work. The created block can
 i
'
J i ( x)

simulate the operation of a gas separation membrane —boundary conditions:

apparatus in three modes: crossflow, direct flow, and
J i (0) = J ci ,
F F
1 countercurrent flow. For each of the modes, a mathe- (7)
matical model of its own is used. The membrane block
is connected to all Aspen Plus thermodynamic pack- J i'(L) = 0, (8)
ages and can be used not only to calculate the mem- —outlet fluxes:
brane process, but also to work in combination with
other processes. JR =  J (L),
i
i (9)

MATHEMATICAL MODEL
OF MEMBRANE MODULE
JP =  J '(0).
i
i (10)

The transfer of gases and vapors through nonpo-
rous polymeric materials is described in terms of the
solution–diffusion mechanism [11]. To calculate mass
transport in the membrane module (Fig. 1), the fol-
lowing equations were used:
In this study, a plate-and-frame membrane mod-
ule was chosen as the object of simulation. This type of
module was designed by Stern [12] and was intended
for the recovery of helium from natural gas on an
industrial scale. The design of the module is similar in

MEMBRANES AND MEMBRANE TECHNOLOGIES Vol. 1 No. 1 2019

 MODELING MEMBRANE GAS SEPARATION
Table 1. Parameters necessary for calculating the model
Input parameter
Component permeability
Membrane area/number of sections
Pressure upstream /downstream of membrane
Feed flux
Concentration of components in feed stream
configuration to that with flat sheet membranes,
which are often used in laboratory experiments in pri-
mary research. The module consists of flat sheet
membranes sandwiching a spacer made from drainage
material [13]. With this design of the module and the
feed stream composition, the crossflow rate becomes
the main parameter that determines the mass trans-
port in the module.
In the study we considered three operating modes
1 of the membrane module: direct flow, countercurrent
flow, and crossflow. Mathematical models of mass
transport for all operation modes are based on the fol-
lowing assumptions: isothermal conditions, the
absence of a pressure gradient in the channel along the
membrane, ideal gas behavior of components, and
constancy of membrane permeability. In the cases of
1 direct and countercurrent flows, the plug-flow mode
is realized in the feed and permeate channels; whereas
the plug-flow mode for crossflow operation is realized
in the feed channel and the flow direction is perpen-
dicular to the membrane in the permeate channel.
CREATING A MODEL OF MEMBRANE GAS
SEPARATION BLOCK IN ASPEN
CUSTOM MODELER
The principle of building a model in ACM is based
on writing equations describing the behavior of com-
ponents or their characteristics in the system under
consideration, for example, material balance equa-
tions, and any necessary additional conditions (for
example, boundary conditions). In the course of
building a model, a certain sequence of actions is
observed. Work on model building begins with the
definition of all parameters and variables involved in
the model. Aspen Custom Modeler has its own exten-
sive database of parameters and variables that can be
selected in the user interface. Next, mathematical
equations are written, which, as a rule, describe the
material and heat balances. The order of the descrip-
tion of a variable or parameter can be studied in the
ACM assistant. To solve the equations, ACM uses
metric units (basic units of measurement); therefore,
the user must ensure that the variables, parameters,
and coefficients in the model equations are written in
basic units. However, the user can select the units for
the variables that are displayed in the graphical user
interface. This means that the values displayed in
MEMBRANES AND MEMBRANE TECHNOLOGIES
3
Output parameter
Retentate/permeate flux
Concentration of components in retentate/permeate
graphs and tables are automatically displayed in the cur-
rent unit of measurement, and the values input into forms
are automatically converted to basic units of measure-
ment. After entering the information about the parame-
ters and variables and spelling out mathematical equa-
tions, streams are connected to the model; in the given
case, the block has three streams: feed stream as the inlet
stream and the retentate and permeate as outlet streams.
In ACM, streams are denoted through ports in which
parameters and variables that carry information, such as
flow temperature, pressure, stream component compo-
sition, and energy characteristics (not considered in this
paper), are built. After the complete information is
defined, the model can be tested. To do this, the compiler
built into ACM is run, which starts the calculation
according to the described model. At this stage, ACM
can identify errors resulting from building the model.
Table 1 lists the parameters necessary for the calculation
of the custom model.
To build a process flowchart using the created
block, the user must have the ACM file in which the
model was created. To export a model from ACM to
Aspen Plus, it is also necessary to have a C++ com-
piler (Visual C ++ package from Visual Studio©) [14].
In order to add the custom block (Fig. 2) to the Aspen
Plus library, it is necessary to enable the option of
export to ACM and then run the import option for this
model in Aspen Plus. Further, the custom model can
be used in the same way as any other elements already
available in the Aspen Plus library.
COMPARISON OF CALCULATION RESULTS
IN ASPEN PLUS WITH EXPERIMENTAL
RESULTS
The calculation block developed was tested on the
basis of comparison of the calculated separation char-
acteristics with available experimental data for the fol-
lowing two cases:
—comparison of the calculation results with the
experimental data obtained upon the separation of the
ternary H2O/EtOH/N2 (13.3/5.5/81.2 mol %) vapor–
gas mixture [15] simulating the stream from the strip-
ping column used in ethanol recovery from fermenta-
tion broth by membrane vapor permeation in a labora-
tory plate-and-frame membrane module, with the
module operating in the countercurrent mode (the 1
experimental part is detailed in [16]);
Vol. 1 No. 1 2019
 4 KOZLOVA et al.

Physicochemical Input parameters

property package and model parameters

ACM user block

Input stream(s) Output stream(s)
J, с, T, P J, с, T, P

C++ compiler
Fig. 2. Scheme of operation of the ACM user block in Aspen Plus.

0.6
Experiment 100
Calculation 90
Concentration of CH4

0.5
in retentate, mol %

80
0.4

Stage cut, %
70
0.3 60
50
0.2 40
30 Experiment
0.1 20 Calculation
0 1
0.0E+00 5.0E–05 1.0E–04 1.5E–04 2.0E–04 0
Feed flow rate, mol/s 0.0E+00 5.0E–05 1.0E–04 1.5E–04 2.0E–04
Feed flow rate, mol/s
Fig. 3. Dependence of the CH4 concentration in the reten-
tate on the feed flow rate. Fig. 4. Dependence of the stage cut on the feed flow rate.

—comparison of the calculation results with exper-
imental data obtained upon the separation of a binary
N2/CH4 (99/1 mol %) [6] gas mixture simulating a stream
with a low concentration of easily penetrating impurity
component using a disk-type membrane module, with the
1 module operating in the countercurrent mode.
The comparison showed that in the case of separa-
tion of the ternary vapor–gas mixture, the calculated
values for the concentrations of the components in the
retentate and permeate streams are basically close to
the experimental values (Table 2). However, a notice-
able deviation is observed for some of them, which can
primarily be due to the influence of longitudinal mix-
ing in the membrane module channels (due to the
presence of the net spacer) and is not taken into
account in mathematical models used for calculation.
In the case of the removal of the easily permeable
impurity component from the binary gas mixture, it
was found that the calculated CH4 concentration in
the retentate is noticeably lower than the experimental
one, especially at low feed flow rates (high stage cuts,
Figs. 3, 4). This is apparently due to the influence of
the longitudinal diffusion (mixing) of components in
the membrane module channels because of a long res-
idence time of the feed upstream of the membrane
(tens of seconds), since the diffusion reduces the sep-
aration characteristics of the membrane apparatus, a
change that is especially noticeable upon the removal

Table 2. Comparison of experimental with calculated results

Component Component concentration Component concentration
Component concentration in feed in permeate, cP, mol % in retentate, cR, mol %
stream, cF, mol % experiment simulation experiment simulation
H2O 13.3% 64.1 ± 4.5% 59.7% 2.8 ± 0.2% 5.2%
EtOH 5.5% 2.7 ± 0.2% 3.0% 6.1 ± 0.4% 6.0%
N2 81.2% 33.2 ± 2.3% 37.3% 91.1 ± 6.4% 88.9%

MEMBRANES AND MEMBRANE TECHNOLOGIES Vol. 1 No. 1 2019

 MODELING MEMBRANE GAS SEPARATION
of impurities and is not taken into account in mathe-
matical models used for the calculation.
In general, the obtained give evidence for the ade-
quacy of the mathematical models used in the gas sep-
aration membrane block developed; the block can be
used to build process flowcharts and analyze the char-
acteristics of separation processes.
CONCLUSIONS
A membrane gas separation unit operating in vari-
ous modes has been developed in the Aspen Plus envi-
ronment for calculating membrane gas separation pro-
cesses. The model built is convenient to export to the
Aspen Plus library, thereby greatly expanding the
capabilities for modeling various processes. The devel-
oped unit makes it possible to perform calculations on
both gas separation and vapor separation membrane
processes. The user is given the opportunity to select
the module operation mode for solving a particular
separation task. A comparison of the results has shown
that the calculated data are close to the experimental
data, confirming that the block can be used for mod-
eling membrane gas separation processes.
LIST OF SYMBOLS
B membrane module width, m
J flow rate upstream of membrane, mol/s
J' flow rate downstream of membrane, mol/s
L membrane module length, m
p pressure upstream of membrane, kPa
p' pressure downstream of membrane, kPa
Q permeability, mol/(m2 s kPa)
с mole fraction
x longitudinal coordinate
SUB/SUPERSCRIPTS
F feed
i component
M membrane
P permeate
R retentate
SPELL: 1. countercurrent
MEMBRANES AND MEMBRANE TECHNOLOGIES
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ACKNOWLEDGMENTS
The work was supported by the Russian Foundation
for Basic Research, project no. 17-38-50100 mol_nr,
and the President of the Russian Federation, grant
no. MK-2924.2017.8.
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Translated by S. Zatonsky
Vol. 1 No. 1 2019