Chemical Engineering and Processing 43 (2004) 11951202

Coupling of ethylbenzene dehydrogenation and benzene hydrogenation

reactions in xed 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 xed 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 xed bed reactor (FBR) with auxiliary reactions achieves substantial increase in ethylbenzene conversion (100%)
compared to the xed 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 reac-
tion is endothermic and reversible with increasing number
of moles. The reaction is severely limited by the thermody-
namic equilibrium with a maximum ethylbenzene conver-
sion 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 modication 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 benets associated with re-
action 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).
well-mixed catalyst patterns in xed 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 ther-
modynamic equilibrium and to supply and remove heat
for endothermic and exothermic reaction systems. The re-
ported results have shown considerable improvement of the
reactors performance [2,10,11]. Despite the evidence of the
catalyst patterns benets, still these congurations 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 xed
bed reactor (FBR). This conguration is different from the
integrated membrane reactor of Moustafa and Elnashaie [7]
and offers many advantages, e.g. the auxiliary reaction is in-
corporated to act as a strong drain-off mechanism alleviating
the equilibrium constraint, a suitable heat integration envi-
0255-2701/$ see front matter 2003 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2003.11.004
1196 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 heteroge-
neous dusty gas model is used which takes into account the
combined ux 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]
C
6
H
5
CH
2
CH
3
C
6
H
5
CHCH
2
+H
2
(1)
r
1
= k
1

P
1
P
2
P
3
K
1

kmol/kg s (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]
C
6
H
6
+3H
2
C
6
H
12
(3)
r
2
= k
2
K
B
P
3
P
4
(1 +K
B
P
4
)(P
3
+P
4
)
kmol/kg s (4)
the rate and equilibrium constants are given by
k
1
= 0.01 exp

0.851
10931.76
T

kmol/kg s kPa (5)

k
2
= 121.11 exp

6038.65
T

kmol/kg s (6)
K
1
= 100.0 exp

122725.157 126.27T
(2.194 10
3
)T
2
RT

kPa (7)
K
B
= 788.0 exp

3019.32
T

kPa
1
(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 xed bed catalytic reactor with
well-mixed catalysts.
of the xed 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 negli-
gible.
4. The catalyst pellet is assumed to be at isothermal steady
state conditions and having slab geometry with charac-
teristic length L
c
[13].
5. Negligible external mass and heat transfer resistances
in the catalyst pellet and the concentration proles are
symmetrical about the center of the pellet.
We consider here a ve-component system(C
8
H
10
, C
6
H
6
,
C
8
H
8
, H
2
, and C
6
H
12
) in which hydrogen participates in
more than one chemical reaction. These components are de-
noted by: 1 for C
8
H
10
, 2 for C
6
H
6
, 3 for C
8
H
8
, 4 for H
2
, and
5 for C
6
H
12
. A differential molar balance on ethylbenzene
and benzene gives
dX
1
dZ
=

1

1
A(1 )zr
1
F
0
1
(9)
dX
2
dZ
=

2

2
A(1 )zr
2
F
0
2
(10)
where X
1
and X
2
are fractional conversions of C
8
H
10
and
C
6
H
6
, respectively,
k
is the volume fraction of catalyst k
and is given by

k
=
volume of catalyst k in a well mixed catalyst bed
volume of a well mixed catalyst bed
,
k =1, 2 (11)
M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202 1197
The molar ow rates of the components at any cross section
of the bed may be written as
F
i
= F
0
i
+
n=2

j=1

ji
F
0
j
X
j
, i = 15 (12)
where
ji
is the stoichiometric coefcient 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:
dP
dZ
= 10
5
(1 )G
0
z
d
P

G
g
c

150
G
(1 )
d
P
+1.75G
0

(13)
3.2. Catalyst pellet and the dusty gas model
The intraparticle mass balance differential equations are
expressed as follows:
dN
i
dl
=
n=2

j=1

ji

j
r
j
, i = 15 (14)
By using the rigorous dusty gas model, the total diffusive
ux can be written as [14,15]
gradC
i
=
N
i
D
e
K
i
+
n=5

j=1,i=j
y
j
N
i
y
i
N
j
D
e
ij
, i = 15 (15)
with the following boundary conditions:
l = 0, N
i
= 0,
l = L
c
, C
i
= C
s
i
, i = 15
(16)
The characteristic length L
c
is given by [13]
L
c
=
V
P
S
P
(17)
where V
P
and S
P
are the volume and external surface area of
the catalyst pellet.The effective diffusivity of any component
(D
e
i
) can be obtained from Eq. (15) by dividing its ux by
the negative of its concentration gradient:
1
D
e
i
=
1
D
e
K
i
+
n=5

j=1,i=j
y
j
y
i
(N
j
/N
i
)
D
e
ij
, i = 15 (18)
The effective molecular diffusivities (D
e
ij
) of the components
are obtained from Wilke equation [14].The effectiveness for
reaction j is given by

j
=

L
c
0
r
j
dL
L
c
r
s
j
, j = 1, 2 (19)
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 subrou-
tine (DGEAR) based on a RungeKuttaVerner fth- and
sixth-order method with automatic step size and double pre-
cision to ensure accuracy. The catalyst pellet equations re-
sulting 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]. De-
tails of the efcient 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 inves-
tigate the effect of the auxiliary reaction. The well-mixed
conguration can be made of composite pellets, i.e. the two
catalysts are co-extruded into composite pellets or two dis-
tinct discrete types of pellets that are physical well-mixed.
In our case, the well-mixed pattern involves loading the re-
actor 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 xed bed reactor
and xed 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
xed 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 xed 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 implement-
ing 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 perfor-
mance of the xed bed reactor is enhanced substantially by
the auxiliary reaction (hydrogenation reaction) and almost
Table 1
Data for the simulation [2,6]
Reactor length 1.0 m
Reactor diameter 2.5 10
2
m
Catalyst pellet diameter 4.75 10
3
m
Porosity of catalyst bed 0.5
Catalyst 1 bulk density 1400 kg/m
3
Catalyst 2 bulk density 1200 kg/m
3
Reaction temperature 873.0 K
Reaction pressure 128.7 kPa
Feed composition (mol%)
Ethylbenzene 50.0
Benzene 25.0
Hydrogen 25.0
1198 M.E.E. Abashar / Chemical Engineering and Processing 43 (2004) 11951202
Fig. 2. Comparison of xed bed reactor (FBR) and xed 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 xed bed reactor with the auxiliary reaction, the hydro-
gen 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 dehydro-
genation and hydrogenation reactions, respectively. It is in-
teresting to note that the drain-off mechanism of hydrogen
alone is sufcient to drive the thermodynamic equilibrium
to high level of conversions.
Fig. 3 shows the ethylbenzene conversion proles along
the reactor length at 873.0 K and different catalyst bed com-
positions. As it can be seen that, although the addition of
catalyst 2 to the bed has signicant impact on improving
the conversion but it can has a negative effect on the reactor
length required for the complete dehydrogenation of ethyl-
benzene. 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
Fig. 3. Ethylbenzene conversion along the reactor for different concen-
trations of catalyst 2.
complete dehydrogenation of ethylbenzene cannot be satis-
ed. 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 tem-
peratures. The proles show a non-monotonic dependence
of exit ethylbenzene conversion on the concentration of cat-
alyst 2. This behavior might be due to the fact that the in-
crease of catalyst 2 in the bed at the expense of catalyst 1.
It is clearly shown that at high temperatures the exit ethyl-
benzene forms plateaus of 100% conversion in wide ranges
of the bed compositions. At relatively low temperatures, the
exit conversions assume maxima with increasing the con-
centration 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 pro-
nounced 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 con-
version for low (T = 750.0 K) and high (T = 873.0 K)
temperatures. As one can see at all pressures the exit con-
version form a maximum at T = 750.0 K. The location of
the maximum is shifted to high bed composition by increas-
ing 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 maxi-
mum may assume an optimum value. At high temperature
(T = 873.0 K), the increase of the pressure has positive ef-
fect on increasing the range of bed composition at which
100% conversion of ethylbenzene is achieved.
The inuence 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 rst composition, (i), is rich in ethylbenzene
and lean in benzene and hydrogen (ethylbenzene: 80 mol%,
benzene: 10 mol%, hydrogen: 10 mol%). The second com-
position, (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 (ethylben-
zene: 10 mol%, benzene: 10 mol%, hydrogen: 80 mol%). For
the fourth composition, (iv), all components have fair rel-
ative amounts (ethylbenzene: 50 mol%, benzene: 25 mol%,
hydrogen: 25 mol%). As it can be seen that the exit conver-
sion is very sensitive to changes in the feed composition. It
is interesting to note that the increase of the temperature has
strong inuence 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%, ben-
zene: 10 mol%, hydrogen: 10 mol%; (ii) ethylbenzene: 10 mol%, ben-
zene: 80 mol%, hydrogen: 10 mol%; (iii) ethylbenzene: 10 mol%, ben-
zene: 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 unied way,
we dened a dimensionless effective reactor length (L
eff
)
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 con-
centration 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.
1200 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 composi-
tion 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 compo-
sition in which the effective length is satised. Within the
start and the end of each range there is an optimum effective
length. The range increases by the increase of the tempera-
ture. It appears that the temperature has a pronounced effect
on the effective length. Increasing the temperature shows a
signicant decrease in the optimum effective length. It is
interesting that the optimum bed composition is not sensi-
tive to changes of the temperature. It is also shown that the
Fig. 8. Effect of catalyst 2 concentration and temperature on the dimen-
sionless effective reactor length.
Fig. 9. Effect of catalyst 2 concentration and pressure on the dimensionless
effective reactor length.
proles 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 effec-
tive reactor length as a function of catalyst 2 composition in
the bed at 873.0 K. Strong inuence 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 phys-
ical intuition. The increase of the pressure favors the hydro-
genation 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 1201
In order to investigate the effect of switching between
low and high temperature beds, the reactor is divided into
two beds. The rst bed is kept at 750.0 K and the second
bed at 900.0 K. The composition of the rst bed and the
second bed is selected as the average optimum composi-
tion of
2
= 0.44 and 0.21 as shown in Figs. 4 and 8,
respectively. The effect of the bed sizes on the ethylben-
zene conversion is shown in Fig. 10. Three volume con-
gurations having volume fractions of 0.3, 0.5, and 0.7
for bed 1 are considered. It is shown clearly that for all
congurations 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 tem-
perature. 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 inuence of hydrogen removal from the reaction
medium by an auxiliary (secondary) reaction on the dehy-
drogenation of ethylbenzene has been investigated in this
work. A rigorous model based on the dusty gas model is
used for the simulation. The inuence 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 reac-
tion). 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 de-
crease 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. Fur-
thermore, 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 xed
bed reactor for ethylbenzene hydrogenation is very promis-
ing. Further theoretical and experimental studies are needed
to investigate different catalyst layer congurations and aux-
iliary reactions.
Appendix A. Nomenclature
A catalyst bed cross-sectional area (m
2
)
C
i
concentration of component i (kmol/m
3
)
d
p
catalyst particle diameter (m)
D
e
i
effective diffusivity of component i (m
2
/s)
D
e
ij
effective molecular diffusivity of component i
(m
2
/s)
D
e
K
i
Knudsen diffusivity of component i (m
2
/s)
g
c
gravitational acceleration (m
2
/s)
G
0
mass velocity of the gas mixture (kg/m
2
s)
F
i
molar ow rate of component i (kmol/s)
F
0
i
initial molar ow rate of component i (kmol/s)
k
1
reaction 1 rate constant (kmol/kg s kPa)
k
2
reaction 2 rate constant (kmol/kg s)
K
1
equilibrium constant of reaction 1 (kPa)
K
B
chemisorption equilibrium constant of benzene
(kPa
1
)
l catalyst pellet coordinate (m)
L
c
characteristic length of the catalyst pellet (m)
N
i
molar ux of component i (kmol/m
2
s)
P
i
partial pressure of component i respectively (kPa)
r
j
rate of reaction j (kmol/kg s)
S
x
external surface area of catalyst pellet (m
2
)
T temperature (K)
V
P
volume of catalyst pellet (m
3
)
X conversion
y mole fraction
z reactor length (m)
Z dimensionless reactor length
Greek letters

k
volume fraction of catalyst k
bed voidage fraction

ji
stoichiometric coefcient for species i in reaction j

j
effectiveness factor of reaction j

G
viscosity of the gas mixture (kg/ms)

i
density of the catalyst i (kg/m
3
)
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