02638762/05/$30.00+0.

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# 2005 Institution of Chemical Engineers
Trans IChemE, Part A, July 2005
Chemical Engineering Research and Design, 83(A7): 811 819

www.icheme.org/journals
doi: 10.1205/cherd.04335

MODELLING AND SIMULATION OF THE MONOLITHIC

REACTOR FOR GAS LIQUID SOLID REACTIONS
T. BAUER1, R. GUETTEL1, S. ROY2, M. SCHUBERT1, M. AL-DAHHAN2 and R. LANGE1

2

1
Department of Chemical Engineering and Process Plant, TU Dresden, Dresden, Germany
Chemical Reaction Engineering Laboratory (CREL), Washington University, St Louis, Missouri, USA

his work provides a mathematical model and process simulations of a monolith

reactor operated in Taylor mode and film flow mode. The three-phase hydrogenation
of a-methylstyrene into cumene and the consecutive hydrogenation of phenyl
acetylene were studied as model reactions. The influences of operating conditions and reactor
parameters, such as superficial gas and liquid velocities, bed structure, pressure and temperature on conversion, selectivity and productivity were examined. This model also includes the
correlations for estimating mass transfer coefficients and kinetic parameters obtained from the
literature. The proposed model has been successfully verified with experimental data. A
comparison of the reactor performance between Taylor flow and film flow under optimum
operating conditions was carried out. Key operating parameters have been identified to maintain optimal performance, which can subsequently be used as criteria for design and scale up.
Furthermore, the behaviour of a trickle-bed reactor was modelled using correlations from the
literature. The simulations for both monolithic and trickle-bed reactors were performed under
optimum operating conditions of each system. It shows that the monolith reactor has higher
selectivity and increased product yield.
Keywords: modelling; monolithic reactor; trickle-bed reactor; hydrogenation; a-methylstyrene; phenyl acetylene.

INTRODUCTION

features especially high mass transfer rates and complete

wetting of the monolith bed. Also, film flow can be
achieved for hydraulic channel diameters greater than
2.0 mm. This regime is similar in flow rates to the trickle
regime in randomly packed reactors, if gas and liquid
flow cocurrently downward through the reactor. A uniform
gas liquid distribution and thus complete wetting of the
bed is more sophisticated due to the low liquid flow rates
(Heibel et al., 2003). The monolithic reactors comprising
the contributions of reaction kinetics, external and intraparticle mass transfer and hydrodynamics have been
studied by different authors. Hatziantoniou and Andersson
(1984) investigated the hydrogenation of nitrobenzoic
acid over palladium catalyst. Besides experimental results
the author proposed a mathematical model for mass transfer
of a monolithic reactor operating in Taylor flow regime.
Irandoust and Andersson (1988) developed a mass transfer
model in which plug flow was assumed in the liquid phase.
Three different mass transfer fluxes (G L, G S, L S)
where considered in the differential mass balance for reacting species. It was found that the model to estimate the
influence of mass transfer predicts the reaction rate quite
reasonably. Cybulski et al. (1993) proposed a mathematical
model for the liquid-phase methanol synthesis. Simulations
showed that the mass transfer is sufficiently fast to allow
the process to be operated in the kinetic regime. Edvinsson

The mini-structured monolith is a promising novel catalyst

carrier for multiphase reactors used in many gas liquid
solid applications, such as hydrogenation, oxidation and
enzymatic reactions. Recently, the current state of development has been reviewed by Roy et al. (2004a) and Boger
et al. (2004). Experimental investigations have revealed
an enhanced performance with respect to mass transfer,
selectivity and conversion. The improvement is mainly
attributed to the more intense gas liquid solid contact
within the regular structure and shorter diffusion distance
due to thin liquid film layer. Depending on superficial gas
and liquid velocities and hydraulic channel diameter, different flow regimes appear within the channels of the substrate
(Simmons et al., 2003). If gas and liquid flow rates are of
the same order of magnitude, with a gas to liquid ratio of
about 0.2 to 2.0 Taylor flow is predominant. An examination of the literature reveals different terms for Taylor
flow, such as slug flow, bubble train flow and so on. In
this study the term Taylor flow is used. This regime


Correspondence to: Professor Dr Lange, Department of Chemical
Engineering and Process Plant, TU Dresden, Muenchner Platz 3, 01062
Dresden, Germany.
E-mail: ruediger.lange@mailbox.tu-dresden.de

811

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BAUER et al.

and Cybulski (1994) compared numerically the performance of a trickle-bed reactor and a monolithic reactor in
terms of space-time yield, selectivity and pressure drop.
Stankiewicz (2001) developed a model for the in-line
monolithic reactor and compared its performance in respect
to mass transfer with a randomly packed reactor. Nijhuis
et al. (2003) evaluated theoretically the performance of a
monolithic reactor and a trickle-bed reactor using the
hydrogenation of styrene. The authors demonstrated that
the monolithic reactor had a three-time higher productivity
while using four-times fewer catalyst. Recently, Roy et al.
(2004b) illustrated a fundamental approach in modelling of
the transport-kinetic interactions in a monolithic catalyst
for operation in film flow mode. However, no studies are
available on whether any comparison between Taylor
flow and film flow modes of operation or any comparison
of monolithic reactors operated in film flow with tricklebed reactors.
The present study provides a mathematical model of the
monolith reactor operated in cocurrent downflow of gas and
liquid for operation in Taylor flow regime and film flow
regime. The proposed model has been validated by comparisons of the calculated results with experimental results.
A comparison of the reactor performance between Taylor
flow and film flow under optimum operating conditions
was carried out. Furthermore, the behaviour of a tricklebed reactor was compared with the monolithic reactor
operated in both Taylor flow regime and film flow
regime. Effect of superficial liquid velocity, flow regime,
monolith geometry, cell density and geometric surface
area has been investigated on the hydrogenation of alphamethylstyrene (AMS) and phenyl acetylene (PA).
REACTOR MODELLING
In order to compare the performance of a monolithic
reactor operated in Taylor and film flow and a tricklebed, reactor models have been developed. The models
were formulated for single pass conversion of the liquid
reactant passing through the reactors. A modified model,
which accounts for multiple-pass flow through the reactor,
was used for the evaluation of model predictions against
experimental data. The partial differential equation systems
for the reactors were solved using the commercial software
tool Aspen Customer Modeler (ACM). The hydrogenation
of a-methylstyrene (AMS) to cumene and the selective
hydrogenation of phenyl acetylene (PA) to styrene were
considered as model reactions.
INTRINSIC KINETICS
The hydrogenation of a-methylstyrene and the consecutive hydrogenation of phenyl acetylene were selected.
The experimental investigation of the kinetics of the hydrogenation of a-methylstyrene was performed by Meille et al.
(2002) and additional details can be found in the associated
publication. The intrinsic reaction rate can be expressed
with the following rate equation:


EA
KH2 cH2
p

r k0  exp 
RT (1 KH2 cH2 )2

(1)

The intrinsic kinetic expressions of the consecutive

hydrogenation of phenyl acetylene has been studied by
Chaudhari et al. (1986), who fitted separately Langmuir
Hinshelwood rate expressions equations (2) and (3). More
details can be found in the related paper.
cH2 cPA
(1 (Kc)PA (Kc)ST )2
cH2 cST
r2 k 2
(1 (Kc)PA (Kc)ST )2

r1 k1

(2)
(3)

GENERAL MODEL ASSUMPTIONS

The developed models for both the monolithic reactor
and the trickle-bed reactor are based on the following
general assumptions: gas and liquid flow in cocurrent
downflow at constant flow rate, isothermal operating condition of the reactors, uniform gas liquid distribution
over the reactor cross-section, liquid components are not
volatile, constant physical properties, operation in steady
state, catalyst effectiveness 100% and no mass transfer
resistance on the gas phase side.
MONOLITHIC REACTOR
The performance of a monolith reactor may be affected
by many factors such as cell density, geometric surface
area, open frontal area, flow regime, interphase mass transfer and intraparticle diffusion. Using the proposed model
allows detailed numerical investigations of these parameters. The mathematical reactor model developed in this
work consists of mass balances of all species in the gas
phase, liquid phase and catalyst layer.
The following particular assumptions are made for the
monolithic reactor: plug flow of fluid phases, no radial
and axial dispersion, active sites are homogeneously distributed in a thin washcoat layer, gas bubbles are approximated by cylinders with spherical ends, the cylindrical
body of the gas bubbles is surrounded by a thin laminar
liquid film between gas and catalyst. Based on the assumptions described, the reactor model is given by the following
set of equations for each phase.
Mass Balances
Gas phase (G)
@cG (H2 , x)
@cG (H2 , x)
uG0
bG
@t
@x



RT
cG (H2 , x)  cL (H2 , x)
 kaGL (H2 )
He(i)



RT
cG (H2 , x)  cS (H2 , x, y)jytwc
 kaGS (H2 )
He(H2 )
(4)
Liquid phase (L)
@cL (i, x)
@cL (i, x)
uL0
bL
@t
@x



RT
cG (i, x)  cL (i, x) (5)
kaGL (i)
He(i)


 kaLS (i) cL (i, x)  cS (i, x, y)jytwc

Trans IChemE, Part A, Chemical Engineering Research and Design, 2005, 83(A7): 811819

MODELLING AND SIMULATION OF THE MONOLITHIC REACTOR

Solid phase (S)
2

1WC

@cS (i, x, y)
@ cS (i, x, y)
Deff (i)
@t
@y2
X

nj (i)rj (x, y)

(6)

Boundary conditions

@cS (i, x, y)
 0
@y
y0

813

The following particular assumptions are made for the

trickle-bed reactor: active sites are uniformly distributed
in the eggshell catalyst layer, radial dispersion is negligible
and the external catalyst surface is partially wetted. The
mathematical reactor model is given by the following
partial differential equations.

Mass Balances
(7)

Boundary condition at external surface of the washcoat

X

0 xWC
hj  nj (i)  rj (x, y)ytWC
j




kaLS (i) cL (i, x)  cS (i, x, y)ytwc




RT
cG (i, x)  cS (i, x, y)ytwc
kaGS (i)
He(i)

(8)

Boundary conditions at the entrance of the reactor

cG (i, x 0) cG (i, x 0 )

(9)

cL (i, x 0) cL (i, x 0 )
i A, B, H2

(10)

The correlations of the geometric, hydrodynamic and

mass transfer parameters used for modelling the reactor
performance in Taylor flow mode are given in Table 1.
The general mass balance equations can be applied also
to describe the monolithic reactor performance for operation in film flow mode. The correlations used for evaluation of the specific parameters for film flow mode are
presented in Table 2.

TRICKLE-BED REACTOR

Gas phase (G)

1G

@cG (H2 , x)
@2 cG (H2 , x)
Dax,G (H2 )
@t
@x2
@(uG cG (H2 , x))
 kaGL (H2 )

@x



RT
cG (H2 , x)  cL (H2 , x)

He(H2 )


RT
cG (H2 , x)
 kaGS (H2 )(1  weff )
He(H2 )

 cS,dry (H2 , x)
(11)

Liquid phase (L)

@(1L cL (i, x))
@2 cL (i, x) @(uL cL (i, x))
Dax, L (i)

2
@t
@x

@x

RT
kaGL (i)
cG (i, x)  cL (i, x)
He(i)
 kaLS (i)weff (cL (i, x)  cS (i, x)) (12)
i A, B
@(1L cL (H2 , x))
@2 cL (H2 , x)
Dax,L (H2 )
@t
@x2
@(uL cL (H2 , x))
kaGL (H2 )

@x



RT
cG (H2 , x)  cL (H2 , x)

He(H2 )

The reactor model applied in this work is based on the

axial dispersion model given by Lange et al. (2004a) to
predict the overall performance of the trickle-bed reactor.

 kaLS (H2 )weff (cL (H2 , x)

 cS,wet (H2 , x))

(13)

Table 1. Correlations used for modelling the monolith reactor in Taylor flow mode.
Parameter
Gasliquid mass transfer
Liquidsolid mass transfer

Gassolid mass transfer

Dimensionless liquid film thickness
Gassolid interfacial area
Liquidsolid interfacial area
Liquid saturation

Correlation

n
1:2
0:133uUC
DA
kaGL
DB
L0,5
L


0:7 !
D
CL
kLS 20
1 0:003
dh
ReUC Sc
kGS

D
df

db,sq
0:7 0:5 exp (2:25Ca0:445 )
dh
4(1  bL )
aGS
dh
4bL
aLS
dh
uL
bL
uL uG

Reference
Bercic and Pintar (1997)
Kreutzer et al. (2001)

Irandoust and Andersson (1988)

Kreutzer et al. (2001)
From geometry
From geometry
Wallis (1969)

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814

BAUER et al.
Table 2. Correlations used for modelling the monolith reactor in film flow mode.

Parameter

Correlation

Gassolid mass transfer

ShGS

kGS df
0:267(1:5z)1:2
3:4145
DL
1 0:2(1:5z)0:7

with: z

Liquid film thickness

Liquid saturation
Gassolid interfacial area
Liquidsolid interfacial area

LR DL
d2f uL

Solid phase (S)

@cS,dry (H2 , x)
kaGS (H2 )(1  weff )
@t



RT
cG (H2 , x)  cS,dry (H2 , x)

He(H2 )
X

nj (H2 )rj,dry
(14)
j

1S

@cS (i, x)
kaLS (i)weff (cL (i, x)  cS (i, x))
@t
X
X

nj (i)rj,wet
nj (i)rj,dry
j

1S

Lebens et al. (1999)

ShLS (1:19 0:0072ReG )1:1 (ReL )0:494 Ga0:22 Sc0:33

u0 r
with: Re
aLS h
s


3 tGL
3 tGL 2
hL
+
df 
3uL0
4 rL g
4 rL g
rL g


2
2df
bL 1  1 
dh
p
4 (dh  2df )dh
aGS
dh2
4
aLS
dh

Liquidsolid mass transfer

1S

Reference

(15)

@cS,wet (H2 , x)
kaLS (H2 )weff (cL (H2 , x)
@t
X
 cS,wet (H2 , x))
nj (H2 )rj,wet (16)

Burghardt and Bartelmus (1996)

VDI Heat Atlas,

Miller and Numrich (1997)
From geometry
From geometry
From geometry

Table 3 lists the correlations used to calculate the model

parameters, which include mass transfer coefficients
[(ka)GL, (ka)LS, (ka)GS], liquid holdup, external liquidsolid contacting efficiency and the axial dispersion.
The employed catalyst and bed characteristics of the
monolithic reactor and trickle-bed reactor as well as the
operating conditions are given in Table 4. The amount of
Pd catalyst is assumed to be one percent of the washcoat
loading. The reactor length is 0.45 m for all three reactor
types considered.
Table 5 gives more detailed specifications about geometric parameters such as cell density x, hydraulic channel
diameter dh, open frontal area OFA and geometric surface
area GSA of the monoliths used in this the study. Furthermore it contains information on the flow regime in which
the gas and liquid moves through the monolith bed,
where FF means film flow and TF means Taylor flow.

RESULTS AND DISCUSSION

Boundary Conditions (Danckwerts Type)

Reactor inlet, x 0

@cL (i, x)
uL (cL (i, x)jx0  cL (i,x)jx0 )
Dax,L (i)
@x x0
(17)

@cG (i, x)
Dax,G (i)
uG (cG (i, x)jx0  cG (i, x)jx0 )
@x x0
(18)

Numerical simulations were performed for both Taylor

flow mode and film flow mode of operation, in which
superficial liquid velocity, cell density and geometric surface area were varied. The effects of these parameters on
conversion, selectivity and productivity are discussed.
Reactor productivity [equation (21)] is described as
follows:
P

DmP
uL0 nA
cA,in MP
XS
tPr oc mcat
LR nP xWC rWC ycat=WC

(21)

i A, B, H2
Reactor outlet, x LR

@cL (i, x)
0
@x xL

@cG (i, x)
0
@x xL
i A, B, H2

(19)
(20)

Equation (21) employs process parameters such as conversion X, selectivity S, superficial liquid velocity uL0 and inlet
concentration of reactant cA0 as well as reactor design
parameters such as reactor length LR and the amount of
catalyst specified with xWC, rWC, ycat/WC. Besides the
often used space time yield, the productivity as well is an
adequate base for comparison of multiphase reactors, as it
considers the amount of product that can be produced in
a certain time by using a defined amount of catalyst.

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MODELLING AND SIMULATION OF THE MONOLITHIC REACTOR

815

Table 3. Correlations used for modelling the trickle-bed reactor.

Parameter

Correlation

Gasliquid mass transfer, hydrogen

Reference

0:46


dR
rL uL 0:14 0:5
ScH2,L
dP
hL

0:82


dR
rL uL 0:9 0:5
kaLS (H2 ) 0:75DH2,L
ScH2,L
dP
hL



r uL 0:56 1=3
Sci,L ; i A, B
kaLS (i) 0:45Di,L L
hL
DH2,G 1=3 1=3
kGS (H2 ) 0:18
1
(1S  1)ReG Sc2=3
H2,G
dP S

0:33
dR
1L 0:16(1  1S )
Re0:14
L
dP



1 (Dp=x)=rL g 1=9
weff 1:104Re1=3
G
GaL
kaGL (H2 ) 0:33DH2,L

Liquidsolid mass transfer, hydrogen

Liquidsolid mass transfer, liquid components
Gassolid mass transfer, hydrogen
Liquid holdup
Wetting efficiency

Lange et al. (1999)

Lange et al. (1999)
Goto and Smith (1975)
Nelson and Galloway (1975)
Lange et al. (2004b)
Al-Dahhan and Dudukovic (1995)

Axial dispersion coefficient, liquid

Dax,L 0:55ReL0:61

Lange et al. (1999)

Axial dispersion coefficient, gas

0:78
Dax,G 13ReG

Lange et al. (1999)

Validation of the Reactor Model

To validate the proposed model for the monolithic reactor the hydrogenation of alpha-methylstyrene was taken as
model reaction. Taylor flow regime is characterized by very
short residence time of the liquids in the reactor and thus
the conversion in a laboratory-scale monolithic reactor is
small. As consequence the experimental setup should be
operated in semi-batch mode with liquid recirculation.
The model predictions for the monolithic reactor operated
in Taylor flow mode are compared with the experimental
results from Roy and Al-Dahhan (2004) at different hydrogen partial pressures. As shown in Figure 1, the model predictions are in good agreement with experimental results,
indicating the applicability of the model over the range of
conditions studied. The dashed line was obtained form
simulations with unpublished kinetic data for this reaction
and conditions.
The good agreement between the experimental results
and model predictions indicates that for the process
conditions applied, the distribution device used in the
experimental setup of Roy Shaibal and Al-Dahhan (2004)
creates a uniform gas-liquid distribution over the reactor
cross-section.

Effect of Liquid Flow Rate and Cell Density on AMS

Conversion and Productivity
The hydraulic diameter of the monolithic channels, the
cell density and the liquid flow rate play a vital role in
the hydrodynamic behaviour, which strongly affects the
conversion and hence the productivity. Figure 2 shows
the effect of superficial liquid velocity on conversion of
AMS at constant gas flow rate. The lowest superficial
liquid velocities applied for both the film flow regime
(FF) and the Taylor flow regime (TF) give highest conversion in the range studied. In general, increase in superficial
liquid velocity results in decrease in conversion. This effect
is more pronounced in the film flow regime than in the
Taylor flow regime. The improved conversion with
decreasing superficial liquid velocity could be mainly
attributed to better mass transfer when liquid film thickness
becomes less with decreasing flow rate. The recirculation
of liquid within the liquid plugs enhances the liquid
solid mass transfer. Hence, the liquid film between the
cylindrical body of the gas bubbles and the catalyst surface
is very thin, which leads to low mass transfer resistance.
This finding is in agreement with the work of Kreutzer
et al. (2001) who investigated mass transfer in Taylor

Table 4. Characteristics of the monolithic reactors and the trickle-bed reactor.

Reactor (flow regime)
Catalyst
Shape
Catalyst type
Washcoat loading [wt%]
Size
External surface area (m2 m23)
Bed void fraction
Conditions
Superficial liquid velocities (m s21)
Superficial gas velocity (m s21)
Temperature (K)
Pressure (bar)

MR (Taylor flow)

MR (film flow)

TBR (trickle flow)

Monolith with square channel shape

Washcoat
10.618.4
Cell density (cpsc): 3193
Wall thickness (mm): 112 213
Washcoat thickness (mm): 14
19293341
0.75

Monolith with square channel shape

Washcoat
3.87.5
Cell density (cpsc): 416
Wall thickness (mm): 313650
Washcoat thickness (mm): 14
6821364
0.75

Pellet
Egg shell
3.3 9.9
Diameter (mm): 2 6
Shell thickness (mm): 14

0.010.5

0.01

0.3
298, 348
15

0.5
298, 348
15

5.3  1023
10.0  1023
0.5
348
15

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600 1800
0.4

816

BAUER et al.

Table 5. Geometric characteristics of the monolithic substrate and flow

regime studied.

x (cpsc)
4
6
8
12
16
31
47
62
78
93

x (cpsi)

dh (mm)

OFA

GSA (m21)

Regime

25
40
50
75
100
200
300
400
500
600

4.40
3.48
3.11
2.54
2.20
1.56
1.27
1.10
0.98
0.90

0.75
0.75
0.75
0.75
0.75
0.75
0.75
0.75
0.75
0.75

682
863
964
1181
1364
1929
2362
2728
3050
3341

FF
FF
FF
FF
FF
TF
TF
TF
TF
TF

flow regime. As seen from Figure 2, film flow regime gives

higher conversion, which could be explained by the longer
residence time of the AMS in the catalyst bed and thus
reducing the time of reaction of AMS with hydrogen at
the catalyst surface.
A direct comparison between Taylor flow and film
flow mode is difficult because of the difference in monolith
substrate geometry and superficial liquid velocity. Therefore productivity was chosen as base of comparison as
it excludes these factors and focuses only on flow rate,
conversion, selectivity and amount of catalyst. Figure 3
illustrates in more detail the influence of superficial liquid
velocity on reactor performance as introduced as productivity. As depicted in Figure 3, Taylor flow gives
higher reactor productivity because of the enhanced mass
transfer characteristic as mentioned earlier. The influence
of gas flow rate is not considered in the numerical simulations. It could be assumed that this effect is not strongly
pronounced and can be neglected.
If only the reactor and the specific catalyst bed are considered, a low liquid velocity leads to high conversion and
thus enhanced product quality for reactor operation in
single pass mode. A superficial liquid velocity of about
0.1 m s21 is almost lowest adjustable velocity for Taylor
flow to guarantee a stable flow regime with enhanced

characteristics. Furthermore, the Taylor flow regime at

higher velocities favours the ratio between the amount of
product and the used amount of catalyst and thus gives
higher productivity.
The next section covers the influence of cell density and
geometric surface are, respectively on conversion and
productivity as shown in Figures 2 and 3.
As can be seen from the Figure 2, significantly higher
conversion was achieved in film flow with monoliths of
low cell density. Hence, conversion gradually increases
with increasing cell density. A four-time increase in cell
density results in almost doubling conversion. The higher
conversion in film flow mode can be accounted to the
low liquid flow rate and thus to the longer residence time
of the liquid reactant within the catalyst bed.
However, it is not possible to infinitely increase the cell
density, because this will reduce the hydraulic diameter and

Figure 1. Monolith reactor performance at elevated pressures: experimental

data and predictions for the hydrogenation of AMS.

Figure 3. Effect of superficial liquid velocity and cell density on reactor

productivity for the hydrogenation of AMS at constant gas flow rate.

Figure 2. Effect of superficial liquid velocity and cell density on AMS

conversion at constant gas flow rate.

Trans IChemE, Part A, Chemical Engineering Research and Design, 2005, 83(A7): 811819

MODELLING AND SIMULATION OF THE MONOLITHIC REACTOR

the channel wall thickness as well. According to findings by
Simmons et al. (2003), a hydraulic channel diameter of at
least 2.0 mm or more is needed to achieve film flow-type
flow introduced as channelling flow in square channels.
The influence of cell density on conversion for reactor
operation in Taylor flow mode is little pronounced. The
figure shows that Taylor flow mode gives almost double
productivity over the range studied. The influence of cell
density is more distinctive in film flow regime.
Film flow achieves higher conversion with lower reactor
length in single pass mode of the reactor. However, the productivity in Taylor flow is always higher compared to film
flow as mass transfer rates are higher in this regime. In
dependency on reactor length or product recirculation,
high conversion can be achieved at the reactor exit. Economically, this leads to an optimization problem in terms of
equipment costs, catalyst costs as well as energy costs for
achieving the desired product quality and quantity.
To guarantee a sufficiently high throughput in film flow
mode of operation, the reactor diameter needs to be
increased. However, an increase in reactor diameter
would mean more sophisticated techniques to achieve uniform gas liquid distribution over the whole cross-section
as described by Heibel et al. (2003). In summary, if high
conversion per pass is desired, the monolithic reactor
could be operated in the film flow regime with monolith
packing of a low cell density and hydraulic channel
diameters greater than 2.0 mm. If product recirculation or
reactor length is not the limiting factor, it is favourable to
operate the reactor in Taylor flow mode with monolithic
packing of high cell density.
Furthermore, the numerical studies revealed that for
Taylor flow with high cell density monolith substrates,
the specific surface area has no impact on selectivity in
contrast with film flow with low cell density monolith
substrates.

817

Figure 4. Effect of specific surface area on PA conversion.

Comparison of Monolithic Reactor and Trickle-Bed

Reactor Performances

monolithic reactor in film flow mode. For reactor operation

in Taylor flow mode, there is no significant influence of
geometric surface area on conversion and selectivity. For
the configuration and conditions studied, it was found
that a monolith with a cell density of 16 cpsc at a superficial
liquid velocity of 0.01 m s21 and a trickle-bed configuration of spherical particles of 3.0 mm operated at a superficial liquid velocity of 0.01 m s21 achieve almost the
same conversion. This could be explained by higher mass
transfer rates from the higher interstitial liquid velocity
within the randomly packed bed.
Figure 6 compares the selectivity at the same conversion
for the trickle-bed reactor and the monolithic reactor in film
flow mode. In general, as illustrated in the figure, the higher
the conversion the lower the selectivity. The most selective
is the film flow regime at the same conversion for the
regimes studied. The trickle-bed reactor with a superficial

A variety of industrial gas liquid solid reaction processes is carried out in trickle-bed reactors, mainly due to
simple assembly and achievement of high catalyst load.
However, pressure drop and the related particle size are
the weak points. To reduce the pressure drop over the
packed bed, larger particles are needed, whereas small particles are desirable for achieving high mass transfer rates
due to the higher specific surface area and short intraparticle diffusion paths. The monolithic structure shoes a very
low pressure drop in consequence of the straight channels
and excellent mass transfer rates. For an evaluation of the
reactor performance, a comparison of both reactor types
is necessary. The effect of specific surface area on the conversion of phenyl acetylene (PA) is shown in Figure 4.
Numerical studies are performed for a monolithic reactor
operated in Taylor flow regime and in film flow regime,
respectively, as well as for a trickle-bed reactor at superficial liquid velocities of 0.5 and 1.0 cm s21. As illustrated
in the Figures 4 and 5, the specific surface area has an
impact on conversion and selectivity. In general, increase
in specific surface area results in increase in catalyst loading, thus enhancement in conversion. This effect is
obviously pronounced for the trickle-bed reactor and

Figure 5. Effect of specific surface area on reactor selectivity for the

hydrogenation of PA.

Trans IChemE, Part A, Chemical Engineering Research and Design, 2005, 83(A7): 811819

818

BAUER et al.
lower conversion than for film flow and trickle flow, so
direct comparability is reduced. The formation of intermediate product increases with increasing conversion and
thus the consecutive reaction is enhanced which lowers
the selectivity towards the intermediate product.
CONCLUSIONS

Figure 6. Selectivity versus conversion for monolithic reactor in film flow

regime and trickle-bed reactor for the hydrogenation of PA.

liquid velocity of 0.01 m s21 shows higher selectivity at the

same conversion as the trickle-bed reactor at a superficial
liquid velocity of 0.005 m s21.
The effect of specific surface area on productivity for the
hydrogenation of PA is shown in Figure 7. In this respect,
the trickle regime and film flow regime are both sensitive to
a change in surface area. Reactor productivity gradually
decreases with increasing surface area. Almost no effect
is observed when the Taylor flow regime is considered.
In summary, film flow and trickle flow have similar productivity at the same superficial liquid velocity. For the criteria applied, it is not obvious which type of reactor is more
suited. Thus only a detailed investment and operation cost
analysis can make a clear distinction. As mentioned earlier,
the Taylor flow mode gives the highest productivity and
best selectivity. Since conversion per reactor length is
low, it needs more effort in plant design regarding total
reactor length and liquid recirculation. It is worth mentioning that the selectivity for Taylor flow is obtained for a

Figure 7. Effect of specific surface area on productivity for the hydrogenation of PA.

The work provides a mathematical model of the monolithic reactor and the trickle-bed reactor as well as numerical process simulations for a range of operating conditions
and reactor configurations. The proposed model was
validated with experimental data obtained from reaction
experiments at different hydrogen partial pressures for
Taylor flow mode. Furthermore, the influence of superficial
liquid velocities, flow regime and bed structures on conversion, selectivity and productivity was studied. It was found
that for the hydrogenation of AMS, film flow gives higher
conversion per pass at same reactor length. However, conversion in Taylor flow regime can be increased if a higher
reactor length or liquid recirculation can be used. Selectivity is also higher in Taylor flow due to lower residence
time, higher mass transfer rates and higher liquid saturation
within the reactor. A comparison between the monolithic
reactor and the trickle-bed reactor has revealed that a
higher conversion can be obtained with the trickle-bed
reactor. But the simulations showed that the monolithic
reactor operated in Taylor flow mode with high cell density
monoliths outperforms the trickle-bed reactor and the
monolithic reactor in film flow mode if selectivity and
productivity are considered. The selection of the type of
reactor and of the flow mode for the monolithic reactor
depends on various factors such as throughput, product
quality and investment costs, and needs optimization for
these parameters in each case.
NOMENCLATURE
a
c
Ca
d
D
Dax
EA
FF
FFMR
g
Ga
GSA
H2
He
k
k
K
L
m
M
MR
OFA
p
Dp
P
PA
r
R
Re
S

specific surface area, m2 m23

concentration, mol m23
capillary number, u . h . d21
diameter, m
diffusion coefficient, m2 s21
axial dispersion coefficient, m2 s21
activation energy, J mol21
film flow
film flow monolithic reactor
acceleration of fall, m s21
Galilei-number, r2 . g . d3k . h22
geometric surface area, m21
hydrogen
Henry coefficient, J mol21
mass transfer coefficient, m s21
kinetic constant, mol m3cat s21
adsorption constant, m3 mol21
length, m
mass, kg
molar weight, kg mol21
monolithic reactor
open frontal area
pressure, Pa
pressure drop, Pa
21
productivity, kgP kg21
cat s
phenyl acetylene
21
reaction rate, mol m23
cat s
gas constant, J mol21 K21
Reynolds-number, r . dk . h21
selectivity

Trans IChemE, Part A, Chemical Engineering Research and Design, 2005, 83(A7): 811819

MODELLING AND SIMULATION OF THE MONOLITHIC REACTOR

Sc
Sh
ST
t
t
T
TBR
TF
TFMR
u
weff
x
x
X
y
y

Schmidt-number, h . r21 . D 21
Sheerwood-number, k . df . D 21
styrene
thickness, m
time, s
temperature, K
trickle-bed reactor
Taylor flow
Taylor flow monolithic reactor
velocity, m s21
wetting efficiency
axial coordinate
volume fraction
conversion
internal coordinate
weight fraction

Greek letters
b
saturation
d
film thickness, m
1
holdup
h
dynamic viscosity, Pa s
h
catalyst effectiveness factor
n
stoichiometric
r
density, kg m23
s
surface tension, N m21
t
shear stress, N m22
z
reciprocal Graetz-number
x
cell density, cpsc
C
dimensionless length, L/dk
Subscripts
0
A
ax
B
b
cat
dry
eff
f
G
GL
GS
h
H2
i
in
j
L
LS
P
P
Proc
R
S
sq
UC
W
WC
wet

superficial
component A
axial
component B
bubble
catalyst
not wetted catalyst surface
effective
film
gas
gasliquid
gassolid
hydraulic
hydrogen
component i
reactor inlet
reaction j
liquid
liquidsolid
particle
product
process
reactor
solid
square
unit cell (one liquid slug and one gas bubble)
wall
washcoat
wetted catalyst surface

819

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ACKNOWLEDGEMENTS
The authors gratefully acknowledge the financial support of the
Chemical Reaction Engineering Laboratory (CREL) and Dresden University of Technology. In addition, two of the authors are grateful to the
Chemical Reaction Engineering Laboratory (CREL) for kind hospitality.
Special thanks to Prof. Dr-Ing. habil. W. Kloden (TU Dresden) for his
valuable suggestions in the handling of ACM.
This paper was presented at the 7th World Congress of Chemical
Engineering held in Glasgow, UK, 1014 July 2005. The manuscript
was received 15 December 2004 and accepted for publication after
revision 18 April 2005.

Trans IChemE, Part A, Chemical Engineering Research and Design, 2005, 83(A7): 811819