Chemical Engineering and Processing 43 (2004) 11951202

Coupling of ethylbenzene dehydrogenation and benzene hydrogenation

reactions in fixed bed catalytic reactors
M.E.E. Abashar
Chemical Engineering Department, College of Engineering, King Saud University, P.O. Box 800, Riyadh 11421, Saudi Arabia
Received 28 April 2003; received in revised form 10 November 2003; accepted 11 November 2003
Available online 29 December 2003

Abstract
The application of dual-functionality via a well-mixed catalyst pattern in an integrated fixed bed catalytic reactor for simultaneous production
of styrene and cyclohexane has been investigated. A rigorous mathematical model based on the dusty gas model is used for the simulation.
Equilibrium shifting is achieved by the drain-off mechanism of hydrogen in dehydrogenationhydrogenation reaction media. The simulation
results show that the fixed bed reactor (FBR) with auxiliary reactions achieves substantial increase in ethylbenzene conversion (100%)
compared to the fixed bed reactor. Optimal conditions are observed and an effective length criterion for the optimal conditions is presented.
The effects of the operating conditions on the reactor performance are examined. It seems that the overall performance of the reactor is a
balance between the operating conditions and the rate of hydrogen removal. The results suggest that appreciable energy saving can be achieved
by maintaining the reactor beds at different temperatures.
2003 Elsevier B.V. All rights reserved.
Keywords: Dual catalyst; Dusty gas model; Fixed bed reactor; Ethylbenzene; Styrene

1. Introduction
Ethylbenzene dehydrogenation over iron oxide catalysts
to styrene is an industrially important chemical reaction [1].
The recent worldwide production of styrene is estimated by
more than 15 million tonnes per year [2,3]. The main reaction is endothermic and reversible with increasing number
of moles. The reaction is severely limited by the thermodynamic equilibrium with a maximum ethylbenzene conversion less than 50% [3]. In this case, the styrene conversion
can be favored by low pressure, high temperature, and the
dilution of the products.
Given the fact that the potential for enhancement of
styrene yield by modification of catalysts appears more or
less limited, considerable effort should be made into the
improvement of the process design [28]. Moustafa and
Elnashaie [7] have shown the benefits associated with reaction coupling in integrated membrane reactors. However,
these integrated membrane reactors still suffer from low
permeation rate of hydrogen. In recent years, spatially or

Fax: +966-1-4678-770.
E-mail address: mabashar@ksu.edu.sa (M.E.E. Abashar).

0255-2701/$ see front matter 2003 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2003.11.004

well-mixed catalyst patterns in fixed bed catalytic reactors

[9] and membrane reactors [10,11] have received increased
attention. The purpose of these patterns (either physically
mixed or layered) is to introduce dual-functionality, i.e. to
introduce auxiliary reactions for further shift of the thermodynamic equilibrium and to supply and remove heat
for endothermic and exothermic reaction systems. The reported results have shown considerable improvement of the
reactors performance [2,10,11]. Despite the evidence of the
catalyst patterns benefits, still these configurations are not
fully understood and the technology is not commercially
utilized.
The purpose of this preliminary investigation is to explore
the advantage gained by dual-functionality of well-mixed
catalyst patterns in shifting the thermodynamic equilibrium
and producing styrene and cyclohexane simultaneously, i.e.
coupling the dehydrogenation reaction of ethylbenzene with
an auxiliary hydrogenation reaction of benzene in a fixed
bed reactor (FBR). This configuration is different from the
integrated membrane reactor of Moustafa and Elnashaie [7]
and offers many advantages, e.g. the auxiliary reaction is incorporated to act as a strong drain-off mechanism alleviating
the equilibrium constraint, a suitable heat integration envi-

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M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

ronment is available and the concept of the catalytic patterns

can be applied. In the present study, a rigorous heterogeneous dusty gas model is used which takes into account the
combined flux relations. Simulation with various parameters
is performed.
2. Reaction kinetics
The kinetics of the main and auxiliary reactions are given
as follows.
2.1. Main reaction
The kinetics of dehydrogenation of ethylbenzene to
styrene on iron-promoted catalysts in the absence of side
reactions is given by [5,6]
C6 H5 CH2 CH3
C6 H5 CHCH2 + H2



P1 P 2 P 3
kmol/kg s
r1 = k1
K1

(1)
(2)

2.2. Auxiliary reaction

The purpose of the auxiliary reaction is the removal of
hydrogen. This may be accomplished through hydrogenation
of benzene on nickel catalysts to cyclohexane. The kinetics
is given by [12]
C6 H6 + 3H2 C6 H12
r2 = k2 KB

(3)

P3 P 4
(1 + KB P4 )(P3 + P4 )

kmol/kg s

(4)

the rate and equilibrium constants are given by


10931.76
k1 = 0.01 exp 0.851
kmol/kg s kPa
T



6038.65
k2 = 121.11 exp
kmol/kg s
T

122725.157 126.27T

(2.194 103 )T 2

K1 = 100.0 exp

RT

(5)
(6)

3019.32
KB = 788.0 exp
T

kPa1

kPa

(7)

(8)

where T is the absolute temperature (K).

3. Model development
3.1. Bulk gas phase
A rigorous one-dimensional heterogeneous model based
on the dusty gas model is developed. A schematic diagram

Fig. 1. Schematic representation of the fixed bed catalytic reactor with

well-mixed catalysts.

of the fixed bed reactor that contains a well-mixed catalyst

pattern is shown in Fig. 1. The following assumptions are
made in the model development:
1. The reactor operates at isothermal steady state conditions
[6].
2. The ideal gas law is obeyed.
3. One-dimensional model, i.e. radial variations are negligible.
4. The catalyst pellet is assumed to be at isothermal steady
state conditions and having slab geometry with characteristic length Lc [13].
5. Negligible external mass and heat transfer resistances
in the catalyst pellet and the concentration profiles are
symmetrical about the center of the pellet.
We consider here a five-component system (C8 H10 , C6 H6 ,
C8 H8 , H2 , and C6 H12 ) in which hydrogen participates in
more than one chemical reaction. These components are denoted by: 1 for C8 H10 , 2 for C6 H6 , 3 for C8 H8 , 4 for H2 , and
5 for C6 H12 . A differential molar balance on ethylbenzene
and benzene gives
1 1 1 A(1 )zr1
dX1
=
dZ
F10

(9)

2 2 2 A(1 )zr2
dX2
=
dZ
F20

(10)

where X1 and X2 are fractional conversions of C8 H10 and

C6 H6 , respectively, k is the volume fraction of catalyst k
and is given by
volume of catalyst k in a well mixed catalyst bed
,
volume of a well mixed catalyst bed
k = 1, 2
(11)

k =

M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

The molar flow rates of the components at any cross section

of the bed may be written as
Fi = Fi0 +

n=2

j=1

ji Fj0 Xj ,

i = 15

(12)

where ji is the stoichiometric coefficient of species i in

reaction j (negative for reactants, positive for products).
The Ergun momentum balance equation is used to give
the pressure drop along the reactor:

0

dP
5 (1 )G z 150G (1 )
0
= 10
+ 1.75G
dZ
dP
dP 3 G gc
(13)
3.2. Catalyst pellet and the dusty gas model
The intraparticle mass balance differential equations are
expressed as follows:
n=2

dNi
ji j rj ,
=
dl

i = 15

(14)

j=1

By using the rigorous dusty gas model, the total diffusive

flux can be written as [14,15]
gradCi =

n=5

yj N i y i Nj
Ni
+
,
e
DKi
Dije

i = 15

(15)

j=1,i=j

with the following boundary conditions:

l = 0,
l = Lc ,

Ni = 0,
Ci = Cis ,

(16)

i = 15

The characteristic length Lc is given by [13]

Lc =

VP
SP

(17)

where VP and SP are the volume and external surface area of

the catalyst pellet.The effective diffusivity of any component
(Die ) can be obtained from Eq. (15) by dividing its flux by
the negative of its concentration gradient:
n=5

yj yi (Nj /Ni )
1
1
=
+
,
e
e
Di
DKi
Dije

i = 15

(18)

j=1,i=j

The effective molecular diffusivities (Dije ) of the components

are obtained from Wilke equation [14].The effectiveness for
reaction j is given by
 Lc
rj dL
, j = 1, 2
(19)
j = 0
Lc rjs
3.3. Solution of the model equations
The ordinary differential equations of the bulk gas phase
(Eqs. (9), (10) and (13)) are integrated by an IMSL subroutine (DGEAR) based on a RungeKuttaVerner fifth- and

1197

sixth-order method with automatic step size and double precision to ensure accuracy. The catalyst pellet equations resulting from using the dusty gas model (Eqs. (14) and (15))
are forming a two-point boundary value problem and solved
by the global orthogonal collocation technique [16]. Details of the efficient computation algorithm developed for
the dusty gas model is given elsewhere [14].

4. Results and discussion

In this study, the well-mixed catalyst pattern in which two
catalysts are involved in the reactions is considered to investigate the effect of the auxiliary reaction. The well-mixed
configuration can be made of composite pellets, i.e. the two
catalysts are co-extruded into composite pellets or two distinct discrete types of pellets that are physical well-mixed.
In our case, the well-mixed pattern involves loading the reactor with two catalysts after physical well-mixed as shown
in Fig. 1.
In order to distinguish between the catalysts employed
in this investigation, the catalyst used for dehydrogenation
of ethylbenzene (the primary reaction) is considered to be
catalyst 1 and that used for the hydrogenation of benzene
(the auxiliary reaction) is catalyst 2. The data used for this
simulation study is shown in Table 1.
Fig. 2a compares the performance of the fixed bed reactor
and fixed bed reactor with the auxiliary reaction (FBR+AR)
at 873.0 K. The ethylbenzene and benzene conversions vary
as functions of the dimensionless reactor length. For the
fixed bed reactor without the auxiliary reaction (1 = 1.00,
2 = 0.00), the ethylbenzene conversion is the same as
the equilibrium conversion, as expected. The performance
of the fixed bed reactor is not satisfactory due to the low
equilibrium conversion (32.96%). The reaction is severely
limited by thermodynamic equilibrium and only small part
of the reactor is utilized. To test the effect of implementing the auxiliary reaction, a small amount of catalyst 2 is
added to catalyst 1 (1 = 0.95, 2 = 0.05) and the mixture
is physically well-mixed. As it can be seen that the performance of the fixed bed reactor is enhanced substantially by
the auxiliary reaction (hydrogenation reaction) and almost
Table 1
Data for the simulation [2,6]
Reactor length
Reactor diameter
Catalyst pellet diameter
Porosity of catalyst bed
Catalyst 1 bulk density
Catalyst 2 bulk density
Reaction temperature
Reaction pressure

1.0 m
2.5 102 m
4.75 103 m
0.5
1400 kg/m3
1200 kg/m3
873.0 K
128.7 kPa

Feed composition (mol%)

Ethylbenzene
Benzene
Hydrogen

50.0
25.0
25.0

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M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

Fig. 3. Ethylbenzene conversion along the reactor for different concentrations of catalyst 2.

Fig. 2. Comparison of fixed bed reactor (FBR) and fixed bed reactor with
the auxiliary reaction ((FBR + AR), 2 = 0.05).

100% conversion of ethylbenzene and benzene is attained.

The corresponding partial pressure of hydrogen along the
length of the reactor is shown in Fig. 2b. For the case of
the fixed bed reactor with the auxiliary reaction, the hydrogen partial pressure passes through a maximum and drops
sharply along the length of the reactor. The occurrence of
the maximum could be due to the balance of simultaneous
formation and consumption of hydrogen by the dehydrogenation and hydrogenation reactions, respectively. It is interesting to note that the drain-off mechanism of hydrogen
alone is sufficient to drive the thermodynamic equilibrium
to high level of conversions.
Fig. 3 shows the ethylbenzene conversion profiles along
the reactor length at 873.0 K and different catalyst bed compositions. As it can be seen that, although the addition of
catalyst 2 to the bed has significant impact on improving
the conversion but it can has a negative effect on the reactor
length required for the complete dehydrogenation of ethylbenzene. This could be due to the fact that the increase of
catalyst 2 in the bed at the expense of catalyst 1. It is also
shown that there exists a bed composition beyond which the

complete dehydrogenation of ethylbenzene cannot be satisfied. It appears that the composition of the bed should be
well controlled.
Fig. 4 shows the exit ethylbenzene conversion varies as
a function of the bed composition for several different temperatures. The profiles show a non-monotonic dependence
of exit ethylbenzene conversion on the concentration of catalyst 2. This behavior might be due to the fact that the increase of catalyst 2 in the bed at the expense of catalyst 1.
It is clearly shown that at high temperatures the exit ethylbenzene forms plateaus of 100% conversion in wide ranges
of the bed compositions. At relatively low temperatures, the
exit conversions assume maxima with increasing the concentration of catalyst 2 in the bed. The maximum is shifted
to the low concentration of catalyst 2 with the increase of

Fig. 4. Exit ethylbenzene conversion vs. catalyst 2 concentration for

various temperatures.

M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

1199

Fig. 5. Effect of catalyst 2 concentration and pressure on exit ethylbenzene

conversion for various temperatures (T = 750.0 and 873.0 K).

the temperature. It appears that the temperature has a pronounced effect on the exit conversion.
In Fig. 5 is shown the effect of changes in the pressure
and catalyst 2 concentration on the exit ethylbenzene conversion for low (T = 750.0 K) and high (T = 873.0 K)
temperatures. As one can see at all pressures the exit conversion form a maximum at T = 750.0 K. The location of
the maximum is shifted to high bed composition by increasing the pressure. It is interesting to observe that the value
of the maximum increases and decreases by increasing the
pressure. The results indicate that the locus of the maximum may assume an optimum value. At high temperature
(T = 873.0 K), the increase of the pressure has positive effect on increasing the range of bed composition at which
100% conversion of ethylbenzene is achieved.
The influence of the feed composition at low (T =
750.0 K) and high (T = 873.0 K) temperatures is presented
in Fig. 6a and b, respectively. Four feed compositions are
considered. The first composition, (i), is rich in ethylbenzene
and lean in benzene and hydrogen (ethylbenzene: 80 mol%,
benzene: 10 mol%, hydrogen: 10 mol%). The second composition, (ii), is rich in benzene and lean in ethylbenzene
and hydrogen (ethylbenzene: 10 mol%, benzene: 80 mol%,
hydrogen: 10 mol%). The third composition, (iii), is rich in
hydrogen and lean in ethylbenzene and benzene (ethylbenzene: 10 mol%, benzene: 10 mol%, hydrogen: 80 mol%). For
the fourth composition, (iv), all components have fair relative amounts (ethylbenzene: 50 mol%, benzene: 25 mol%,
hydrogen: 25 mol%). As it can be seen that the exit conversion is very sensitive to changes in the feed composition. It
is interesting to note that the increase of the temperature has
strong influence on case (ii) and (iv) as shown in Fig. 6b.
As it has been shown in Fig. 3 that there is a wide range of
bed composition, which gives 100% conversion of ethylben-

Fig. 6. Effect of catalyst 2 concentration and feed composition on exit

ethylbenzene conversion. Conditions: (i) ethylbenzene: 80 mol%, benzene: 10 mol%, hydrogen: 10 mol%; (ii) ethylbenzene: 10 mol%, benzene: 80 mol%, hydrogen: 10 mol%; (iii) ethylbenzene: 10 mol%, benzene: 10 mol%, hydrogen: 80 mol%; (iv) ethylbenzene: 50 mol%, benzene:
25 mol%, hydrogen: 25 mol%. (a) T = 750.0 K; (b) T = 873.0 K.

zene at different reactor lengths and in some cases far from

the reactor exit, i.e. at shorter reactor lengths. Therefore, in
order to investigate the reactor performance in a unified way,
we defined a dimensionless effective reactor length (Leff )
as the length of the reactor that gives 99.85% conversion
of ethylbenzene. Fig. 7 shows the effective reactor length
versus the bed composition at 873.0 K. It is shown that the
effective length passes through a minimum with increasing
catalyst 2 in the bed. The occurrence of the minimum could
be due to the interaction of many factors such as the concentration of the catalysts in the bed, temperature, pressure,
and the thermodynamic equilibrium. This result indicates
that the composition of the catalyst bed should be controlled
carefully.

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M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

Fig. 7. Dimensionless effective reactor length as a function of catalyst 2

concentration.

Sensitivity analysis for the effect of the temperature on

the effective reactor length as a function of bed composition at P = 128.7 Pa is shown in Fig. 8. As it can be seen
that for each temperature there is a range of bed composition in which the effective length is satisfied. Within the
start and the end of each range there is an optimum effective
length. The range increases by the increase of the temperature. It appears that the temperature has a pronounced effect
on the effective length. Increasing the temperature shows a
significant decrease in the optimum effective length. It is
interesting that the optimum bed composition is not sensitive to changes of the temperature. It is also shown that the

Fig. 8. Effect of catalyst 2 concentration and temperature on the dimensionless effective reactor length.

Fig. 9. Effect of catalyst 2 concentration and pressure on the dimensionless

effective reactor length.

profiles are not symmetric about the optimum composition

and the effective length is more sensitive to temperature and
bed composition on the right hand side of the optimum bed
composition. It is clearly shown that the effective length is
more sensitive to temperature changes at low temperatures
that at high temperatures.
Fig. 9 shows the effect of operating pressure on the effective reactor length as a function of catalyst 2 composition in
the bed at 873.0 K. Strong influence of the pressure on the
effective reactor length is shown. It is clear shown that the
minima are shifted to the right, i.e. to high concentration of
catalyst 2 in the bed. This result is consistent with the physical intuition. The increase of the pressure favors the hydrogenation reaction of benzene due to decrease in number of
moles (Eq. (3)).

Fig. 10. Two beds at different temperatures.

M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202

In order to investigate the effect of switching between

low and high temperature beds, the reactor is divided into
two beds. The first bed is kept at 750.0 K and the second
bed at 900.0 K. The composition of the first bed and the
second bed is selected as the average optimum composition of 2 = 0.44 and 0.21 as shown in Figs. 4 and 8,
respectively. The effect of the bed sizes on the ethylbenzene conversion is shown in Fig. 10. Three volume configurations having volume fractions of 0.3, 0.5, and 0.7
for bed 1 are considered. It is shown clearly that for all
configurations the switching policy achieves almost 100%
conversion of ethylbenzene. It appears that is possible to
achieve high conversion of ethylbenzene by switching from
a long bed at low temperature and a short bed at high temperature. This is very interesting results, since it is known
that excessive temperatures have destructive effects on
the catalysts and the mechanical stability of the reactors.
Moreover, the energy operating cost is high at elevated
temperatures.

5. Conclusions
The influence of hydrogen removal from the reaction
medium by an auxiliary (secondary) reaction on the dehydrogenation of ethylbenzene has been investigated in this
work. A rigorous model based on the dusty gas model is
used for the simulation. The influence of several operating
parameters has been studied numerically. In the range of the
parameters investigated, the simulation results reveal that
very large increases in the conversion of ethylbenzene can
be realized via equilibrium shifting of the dehydrogenation
reaction of ethylbenzene (primary reaction) when coupled
with hydrogenation reaction of benzene (secondary reaction). The overall performance of the reactor is shown to be
a balance between the operating conditions and the rate of
hydrogen removal. Effective operating regions with optimal
conditions are observed. It is found that substantial decrease in the reactor length is achievable by employing the
dual-functionality of the catalyst mixture. The results also
suggest that appreciable energy saving can be achieved by
maintaining the reactor beds at different temperatures. Furthermore, several products can be obtained simultaneously,
e.g. styrene and cyclohexane.
The results present here are indicative feasibility, which
show that the introduction of dual-functionality into a fixed
bed reactor for ethylbenzene hydrogenation is very promising. Further theoretical and experimental studies are needed
to investigate different catalyst layer configurations and auxiliary reactions.

Appendix A. Nomenclature
A
Ci

catalyst bed cross-sectional area (m2 )

concentration of component i (kmol/m3 )

dp
Die
Dije
e
DK
i
gc
G0
Fi
Fi0
k1
k2
K1
KB

l
Lc
Ni
Pi
rj
Sx
T
VP
X
y
z
Z

1201

catalyst particle diameter (m)

effective diffusivity of component i (m2 /s)
effective molecular diffusivity of component i
(m2 /s)
Knudsen diffusivity of component i (m2 /s)
gravitational acceleration (m2 /s)
mass velocity of the gas mixture (kg/m2 s)
molar flow rate of component i (kmol/s)
initial molar flow rate of component i (kmol/s)
reaction 1 rate constant (kmol/kg s kPa)
reaction 2 rate constant (kmol/kg s)
equilibrium constant of reaction 1 (kPa)
chemisorption equilibrium constant of benzene
(kPa1 )
catalyst pellet coordinate (m)
characteristic length of the catalyst pellet (m)
molar flux of component i (kmol/m2 s)
partial pressure of component i respectively (kPa)
rate of reaction j (kmol/kg s)
external surface area of catalyst pellet (m2 )
temperature (K)
volume of catalyst pellet (m3 )
conversion
mole fraction
reactor length (m)
dimensionless reactor length

Greek letters
k
volume fraction of catalyst k

bed voidage fraction

ji stoichiometric coefficient for species i in reaction j
j
effectiveness factor of reaction j
G viscosity of the gas mixture (kg/m s)
i
density of the catalyst i (kg/m3 )
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