CFD of A Catalytic Micro-Monolith

INTERNATIONAL JOURNAL OF CHEMICAL
REACTOR ENGINEERING
Volume 9 2011 Article A21
CFD Modeling and Simulation of a
Catalytic Micro-Monolith
Almerinda Di Benedetto
Valeria Di Sarli
National Research Council, dibenede@irc.cnr.it
National Research Council, disarli@irc.cnr.it

ISSN 1542-6580
Copyright c 2011 The Berkeley Electronic Press. All rights reserved.
CFD Modeling and Simulation of a Catalytic
Micro-Monolith
Almerinda Di Benedetto and Valeria Di Sarli
Abstract
In this work, a rst step in modeling and simulating the thermal behavior of
an entire catalytic micro-monolith was performed. In particular, a Computational
Fluid Dynamics (CFD) model was developed for simulating three-channel and
ve-channel micro-combustors. For both congurations, the operating maps were
built as functions of the inlet gas velocity and compared to the operating map of a
single-channel conguration.
Results show that, due to the relevance of heat losses in micro-devices, it is not
possible to extrapolate the behavior of the multi-channel congurations from that
of the single channel. Therefore, simulation of the entire catalytic micro-monolith
is needed. However, this is computationally demanding: it has been found that the
CPU time almost linearly increases with the number of channels simulated.
Finally, for a xed total mass ow rate, it has been demonstrated the opportunity
to maximize the overall fuel conversion by means of a non-uniform distribution
of mass ow rates among the channels.
KEYWORDS: catalytic micro-monolith, multi-channel conguration, CFD
1. Introduction

Catalytic monoliths are continuous structures made of a large number of straight
parallel and thin channels with walls coated by catalyst. They are used in many
practical applications, especially those involving oxidation of hydrocarbons in fast
heterogeneous reactions (see, e.g., Hayes and Kolaczkowski, 1994; Groppi et al.,
1999; Dons et al., 2002).
Nowadays, a further relevant application has been proposed in micro-
electro-mechanical-systems (MEMS). In such application, micro-scale monoliths
are used to promote catalytic combustion in channels with typical values of the
diameter equal to around 600 m. Catalytic micro-combustors have to face the
issues of thermal management and control in order to achieve stable steady-state
conditions, prevent extinction and blow-out, and avoid hot spots, traveling heat
waves and wrong way behaviors.
Due to the geometry scale, catalytic micro-combustors do not lend
themselves easily to detailed experimental diagnostics for measurements of
temperature, concentration and velocity fields. Therefore, designing such micro-
combustors is mainly pursued by means of mathematical modeling and
simulation.
Modeling catalytic monoliths can be performed at different scales:
catalyst, single-channel, multi-channel and entire reactor scale. For catalytic
macro-combustors, models have been developed at all relevant scales: from the
catalyst scale, to the single-channel, multi-channel and reactor scales (see, e.g.,
Kolaczkowski and Worth, 1995; Jahn et al., 1997; Jeong et al., 2002; James et al.,
2003; Tischer and Deutschmann, 2005; Di Benedetto et al., 2006; Mei et al.,
2006). It has been demonstrated that modeling a single channel of the monolith
can be inadequate when the effects of non-uniform distribution at the inlet
section, catalyst deactivation and/or heat losses toward the external environment
are relevant (Kolaczkowski and Worth, 1995; Jahn et al., 1997; Jeong et al., 2002;
James et al., 2003; Mei et al., 2006).
The literature models for catalytic micro-combustors are based on the
single-channel assumption (see, e.g., Spadaccini et al., 2007; Kaisare et al., 2008;
Di Benedetto et al., 2009; 2010a; 2010b). It has been widely shown that the
thermal management in such reactors is crucial, especially with regard to the role
of heat losses toward the external environment. This issue limits the application of
catalytic micro-combustors to low values of inlet gas velocities and, thus, input
power densities.
1 Di Benedetto and Di Sarli: CFD of a Catalytic Micro-Monolith
Published by The Berkeley Electronic Press, 2011
to the operating map of a single-channel configuration.

To this end, a continuation analysis was performed by means of direct
Computational Fluid Dynamics (CFD) simulations of the catalytic micro-reactor.
We started from a stable steady-state solution and then continued the solution
branch changing the inlet gas velocity, eventually building the entire operating
map for the catalytic micro-combustor.
Furthermore, for a fixed value of total mass flow rate, the opportunity to
feed the channels of the five-channel micro-combustor with different mass flow
rates was investigated in order to maximize the global fuel conversion and, thus,
the output power density.

2. The Model

A two-dimensional CFD model was developed to simulate the coupling of the
fluid flow and the chemical processes at the gas-solid interface and in the gas
phase for lean propane/air combustion. Figure 1 shows the schemes of the
catalytic micro-combustors with three (A) and five (B) channels.
Each channel consists of two parallel (infinitely wide) plates (gap
distance, d = 600 m; wall thickness, d
w
= 200 m; total length, L = 10 mm). The
schemes of Figure 1 are symmetric (the dashed line is the symmetry line).
Therefore, the computational domain corresponds to the half of each scheme.
For each channel, the model solves the mass, momentum, chemical
species and energy conservation equations in the fluid, along with the energy
equation in the solid wall. Steady-state computations were carried out.

In this work, a first step in modeling and simulating the thermal behavior
of an entire catalytic micro-monolith was performed. In particular, we focused on
three-channel and five-channel micro-combustors. For both configurations, we
built the operating maps as functions of the inlet gas velocity, and compared them
2 International Journal of Chemical Reactor Engineering Vol. 9 [2011], Article A21
http://www.bepress.com/ijcre/vol9/A21

Figure 1 Schemes of the catalytic micro-combustors with three (A) and five (B)
channels.

d
d
w
L
v
in
, T
in
, y
in
wall_1
wall_2
wall_4
wall_3
A
d
d
w
L
v
in
, T
in
, y
in
wall_1
wall_2
wall_4
wall_3
wall_6
wall_5
B
The conservation equations in the fluid are listed below (conventional

notation is adopted):

Continuity

0 =
|
|
.
|
\
|
c
c
+
c
c
+
c
c
+
c
c
y
v
x
v
y
v
x
v
y
x
y x

(1)

Momentum

y x x
p
y
v v
x
v v
yx
xx
y x
x x
c
c
+
c
c
+
c
c
=
c
c
+
c
c
t
t
(2)

y x y
p
y
v v
x
v v
yy xy y y y x
c
c
+
c
c
+
c
c
=
c
c
+
c
c t t
(3)

Species (i = 1,....., N
s
- 1, with N
s
species number)

, , ,
y i
x i i i
i m i m Hom i
v Y
v Y Y Y
D D R
x y x x y y

c
| | c c c c c | |
+ = + +
| |
c c c c c c
\ .
\ .
(4)

Energy

,
,
,
1 1
S S
y
x
i
i
i i m
N i i m N
i Hom i
i i
v h
v h T T
x y x x y y
Y
Y
h D
h D
y
x
h R
x y
= =
c | | | | c c c c c
+ = + +
| |
c c c c c c
\ . \ .
| | | | c
c | |
c
c
| |
|
c
c
\ . \ .
|
+ +
|
c c
|
\ .

(5)

The above equations are coupled to the ideal-gas equation:

mix
pW
T
=
9
(6)


|
|
.
|
\
|
c
c
+
c
c
=
2
2
2
2
0
y
T
x
T
w w
w
(7)

where
w
is the solid thermal conductivity.
Concerning the boundary conditions, at the central line of the
configurations (dashed line in Figure 1), a condition of symmetry was assigned.
At the inlet of each channel, a fixed flat velocity profile was assumed. For
chemical species and energy, Danckwerts boundary conditions were used. At the
exit, the static pressure was imposed as equal to the atmospheric pressure, and far-
field conditions were specified for the remaining variables.
At the fluid-wall interface, a no-slip boundary condition was assigned (the
fluid has zero velocity relative to the boundary) which was coupled to the species
balances (the mass flux of each species, J
i
, is equal to its rate of
production/consumption, e
y,i
):

i y ,i
J e =
(8)

and the energy balance:

w
w h
T T
y y
e
c c
= +
c c
(9)

where e
h
is the heat surface production rate.
Heat losses from the ends of the channels were not considered (insulated
ends), while Newtons law of convection was used at the outer surface of the
external channels:

( )
w,ext a,ext
q h T T =
(10)

where h is the exterior convective heat transfer coefficient, T
w,ext
is the
temperature at the exterior wall surface, and T
a,ext
is the external temperature
(= 300 K).
The energy equation in the solid wall reads as follows:

( ) ( )
3 8 2
0 1 1 65 . .
v C H O
1.256 E 8
R 4.836 E 9 exp C C
T
+ | |
= +
|
9
\ .
3
kmol
m s
| |
|
\ .

(11)

where the activation energy is in J/kmol and the concentrations in kmol/m
3
.
The catalytic reaction was assumed to be irreversible, first order in fuel
concentration and zeroth order in oxygen concentration (Spadaccini et al., 2007).
The reaction rate, referred to platinum as the catalyst, was calculated according to:

3 8
9 06
cat C H
. E 7
R 2.4 E 5 exp C
T
+ | |
= +
|
9
\ .

2
kmol
m s
| |
|
\ .
(12)

where the activation energy is in J/kmol and the concentration in kmol/m
2
.
The molecular viscosity was approximated through Sutherlands law for
air viscosity. The fluid specific heat and thermal conductivity were calculated by
a mass fraction weighted average of species properties. The species specific heat
was evaluated as a piecewise fifth-power polynomial function of temperature.
The model equations were discretized using a finite volume formulation
on a uniform structured mesh. Grid-independent solutions were found with a cell
size equal to 2.5 E-2 mm.
The spatial discretization of the model equations used second order central
differences. Computations were performed by means of the segregated pressure-
based solver of the CFD code ANSYS
Fluent 6.3 (www.fluent.com). The

SIMPLE method was used for treating pressure-velocity coupling. All residuals
were always smaller than 1.0 E-7.
The operating and initial conditions for simulations are summarized in
Table 1 and Table 2, respectively.

The reaction rate for homogenous (volumetric) propane combustion was
calculated according to the single-step reaction rate by Westbrook and Dryer
(1981):
Table 1 Operating conditions for simulations

Parameter Value
Inlet gas temperature, T
in
(K) 300
Inlet gas velocity, v
in
(m/s) Varies
Inlet propane mole fraction, Y
C3H8,in
0.024
Exterior convective heat transfer
coefficient, h (W/m
2
K)
20
Pressure, p (bar) 1
Solid thermal conductivity,
w
(W/m K) 2

Table 2 Initial conditions for simulations
Parameter Value
Gas temperature, T (K) 750
Gas velocity, v (m/s) 0.5
Propane mole fraction, Y
C3H8
0.024
Wall temperature, T
wall
(K) 750
Pressure, p (bar) 1

In Table 3, the values of the non-dimensional numbers Da
1
, Da
2
and Pe
are given as calculated according to Spadaccini et al. (2007) in the range of inlet
gas velocities investigated. These values suggest that the diffusion of reactants is
controlling (the reaction time is two orders of magnitude smaller than the
diffusion time) and that reactants have enough time to contact the catalytic surface
(the diffusion time is of the same order as the residence time).

Table 3 Ranges for Da
1
, Da
2
and Pe
Non-dimensional number Range
Da
1
=
residence
reaction
t
t

~ 400 - 900
Da
2
=
diffusion
reaction
t
t

~ 100
Pe =
diffusion
residence
t
t

~ 0.1 - 0.3
3. Results and Discussion

In Figure 2, the propane conversion is plotted versus the inlet gas velocity as
computed at the outlet section of all three configurations investigated. The 95 %
conversion line is also shown in the figure (dashed line). It can be observed that
the range of inlet gas velocities with conversion higher than 95 % increases in
going from the single-channel (1_C) to the three-channel (3_C) and to the five-
channel (5_C) configuration. The reason for this behavior can be found in the
different temperature level and, thus, degree of adiabaticity established inside the
channels of the three configurations.

Figure 2 Propane conversion versus the inlet gas velocity as computed at the
outlet section of the three configurations investigated (the 95 % conversion line is
also shown).

In Figure 3, the axial profiles of the wall temperature of the central
channel are shown as obtained for different configurations. The maximum wall
temperature for the multi-channel (3_C and 5_C) configurations is about 600 K
higher than that found with the 1_C configuration. The advantage of higher
propane conversions provided by the multi-channel configurations is
v
in
(m/s)
1 10
C
o
n
v
e
r
s
i
o
n

o
f

C
3
H
8

(
%
)
20
40
60
80
100
1_C
3_C
5_C
95 % conversion
counterbalanced by the drawback of higher wall temperatures that are not

sustainable by the catalyst.

Figure 3 Axial profiles of the wall temperature of the central channel as
obtained for the three configurations investigated (v
in
= 0.5 m/s).

In Figure 4, the temperature maps are presented for the three
configurations. The figure shows that also the external channels (not only the
internal ones) of the 3_C and 5_C configurations are hotter than the single
channel. This can be attributed to the fact that the external channels are protected
by the adjacent channels in which heat is produced and stored. It is also worth
noting the presence of a hot spot inside the internal channels. The hot spot
demonstrates the occurrence of the homogeneous reaction that allows completing
the propane conversion.

Central Channel
x (m)
0.000 0.002 0.004 0.006 0.008 0.010
T
w
a
l
l

(
K
)
900
1050
1200
1350
1500
1650
1800
3_C
1_C
5_C

Figure 4 Temperature (K) maps for the three configurations investigated
(v
in
= 0.5 m/s).

In Figure 5, the maps of the homogeneous (volumetric) reaction rate (R
v
)
are reported as obtained for the three configurations investigated. It is shown that,
due to the different boundary conditions, the external channels of both the 3_C
and 5_C configurations exhibit asymmetric profiles: the homogeneous reaction
front starts from the internal wall, which is hotter, and then propagates along the
channel, thus activating the reactive process also at the external wall.

T
1_C
3_C
5_C

Figure 5 Maps of the homogeneous (volumetric) reaction rate (R
v
) for the three
configurations investigated (v
in
= 0.5 m/s).

In Figure 6, the axial profiles of the heat exchanged toward the external
environment (heat losses) per unit volume are shown as computed for the three
configurations. It can be observed that the heat losses per unit volume are much
higher in the case of the single channel. This result confirms the higher level of
adiabaticity of the multi-channel configurations.

R
v
(kmol/ m
3
s)
5_C 3_C 1_C
3_C
5_C
1_C

Figure 6 Axial profiles of the heat losses per unit volume as computed for the
three configurations investigated (v
in
= 0.5 m/s).

From the above-presented results, it is clear that the behavior of the multi-
channel configurations cannot be extrapolated from the behavior of the single
channel. Therefore, the full scale of the catalytic micro-monolith should be
modeled and simulated. The main drawback of such an approach is the
computational cost. Table 4 gives the CPU times for a single iteration required by
the simulations of the three configurations (minimal variations for the CPU times
were found between iterations).

Table 4 CPU times for a single iteration required by the simulations of the three
configurations
Configuration CPU time (s)
1_C 0.1
3_C 0.26
5_C 0.47

x (m)
0.000 0.002 0.004 0.006 0.008 0.010
H

(
W
/
m
3
)
-25
-20
-15
-10
-5
0
3_C
5_C
1_C
The CPU times for the 3_C and 5_C configurations are around three and
five times higher, respectively, than the CPU time needed by the 1_C
configuration.

3.1 Blow-Out

Figure 2 shows that, for the 5_C configuration, the propane conversion
significantly decreases starting from v
in
= 1.67 m/s. This suggests the occurrence
of blow-out: the residence time is too low and, therefore, the reaction front is
swept out of the reactor.
In Figure 7, the maps of the homogeneous reaction rate are shown as
obtained at different inlet gas velocities (v
in
) for the 5_C configuration. When the
inlet velocity is increased, the homogeneous reaction front shifts downstream: it
first exits the external channels (v
in
= 1.67 m/s) and then the internal channels
(v
in
= 2 m/s). The external channels exchange heat with the environment and,
therefore, are colder. On the contrary, the internal channels are more adiabatic.

Figure 7 Maps of the homogeneous reaction rate (kmol/m
3
s) as obtained at
different inlet gas velocities (v
in
) for the 5_C configuration.

In Figure 8, the homogeneous and heterogeneous reaction rates are plotted
versus the axial position for all channels of the 5_C configuration. The
homogeneous reaction rate was calculated at the central line of each channel, the
heterogeneous reaction rate at wall_1, wall_3 and wall_5 (Figure 1B). The figure
shows that, when the inlet gas velocity is increased, the homogeneous and
heterogeneous reaction fronts move along the channel up to reach the exit.
v
in
= 0.5 m/s v
in
= 1.5 m/s
v
in
= 2 m/s v
in
= 1.67 m/s

Figure 8 Axial profiles of the homogeneous (R
v
) and heterogeneous (R
cat
)
reaction rates at different inlet gas velocities (v
in
) for the 5_C configuration.
v
in
= 2 m/s
x (m)
0 2e-3 4e-3 6e-3 8e-3 1e-2
R
v

(
k
m
o
l
/
m
3

s
)
0.0
0.2
0.4
0.6
R
c
a
t

(
k
m
o
l
/
m
2

s
)
1e-7
1e-6
1e-5
1e-4
1e-3
v
in
= 1.67 m/s
R
v

(
k
m
o
l
/
m
3

s
)
0.0
0.5
1.0
1.5
R
c
a
t

(
k
m
o
l
/
m
2

s
)
1e-7
1e-6
1e-5
1e-4
1e-3
v
in
= 1.5 m/s
R
v

(
k
m
o
l
/
m
3

s
)
0.0
0.5
1.0
1.5
R
c
a
t

(
k
m
o
l
/
m
2

s
)
1e-7
1e-6
1e-5
1e-4
1e-3
v
in
= 0.5 m/s
R
v

(
k
m
o
l
/
m
3

s
)
0.0
0.5
1.0
1.5
R
c
a
t

(
k
m
o
l
/
m
2

s
)
1e-7
1e-6
1e-5
1e-4
1e-3
wall_1
wall_3 wall_5
central middle external

In Table 5, the propane conversion attained at the outlet section of each
channel of the 5_C configuration is given for different inlet gas velocities. The
values reported in the table confirm that, when the homogeneous and
heterogeneous reaction fronts are blown out, the global propane conversion
becomes lower than 100 %.

Table 5 Propane conversion attained at the outlet section of each channel of the
5_C configuration at different inlet gas velocities
v
in
(m/s)
Central
channel
Middle
channel
External
channel
0.5 100 100 100
1.5 100 100 100
1.67 100 100 91
2 85 84 71

3.2 Effect of Inlet Velocity Distribution

One of the main challenge for catalytic micro-combustors is to extend their
operability region. This region can be defined as the operative parameter zone in
which the fuel conversion is higher than 95 % (Kaisare et al., 2008). By enlarging
the range of inlet gas velocities at which the micro-combustor achieves a fuel
conversion higher than 95 %, it is possible to operate at higher power densities.
From the above-presented results, it can be concluded that, in the multi-
channel configurations, the central channel is more adiabatic and then has a larger
operability map in terms of inlet gas velocities. In particular, the critical value of
inlet velocity (uniform feeding among the channels) for achieving 95 % propane
conversion in the 5_C configuration is equal to 1.64 m/s (global value equal to
8.2 m/s).
We performed simulations by feeding the channels of the 5_C
configuration with different inlet gas velocities to identify the optimal feeding
conditions, i.e., the conditions that allow maximizing the power density. In
particular, we fixed the total inlet flow rate (i.e., the total inlet velocity = 8.2 m/s),
but changed the feeding distribution among the channels. Table 6 summarizes the
conditions investigated.

Table 6 Inlet gas velocity (m/s) distributions for the 5_C configuration
Configuration
External
channel
Middle
channel
Central
channel
Middle
channel
External
channel
A 1.4 1.8 1.8 1.8 1.4
B 1.64 1.64 1.64 1.64 1.64
C 1.1 2 2 2 1.1
D 1.5 1.6 2 1.6 1.5
E 1.15 1.7 2.5 1.7 1.15

In Figure 9, the overall propane conversions as computed for the inlet
velocity distributions of Table 6 are shown. It can be observed that the optimal
configuration is configuration A in which complete propane conversion is
achieved.

Figure 9 Overall propane conversions as computed for the inlet velocity
distribution reported in Table 6.

v
in
(m/s)
0 2 4 6 8
C
3
H
8

c
o
n
v
e
r
s
i
o
n

(
%
)
89
93
94
97
100
A
C
B
D
external channel
middle channel
central channel middle channel
external channel
E
In Figure 10, the maps of the homogeneous reaction rate are shown for
configurations A, B and E of Table 6.

Figure 10 Maps of the homogeneous reaction rate (kmol/m
3
s) for
configurations A, B and E of Table 6.

A
B
E
With configuration A, the homogeneous reaction front is stabilized inside

each channel. The occurrence of this reaction allows completing the propane
conversion. Conversely, with configuration B, the homogeneous reaction front is
stabilized only inside the internal channels, whereas is swept out of the external
channels due to heat losses, which become predominant with respect to heat
production. Under these conditions, the propane conversion for the external
channels does not complete and, therefore, the overall conversion is lower. With
configuration E, the homogeneous reaction front is stabilized inside all channels,
except for the central channel. In this case, the reaction front is blown out due to
the too high inlet velocity (v
in
= 2.5 m/s) and then too low residence time.
From these results, it is clear that, depending on the channel position,
different inlet gas velocities can be used, thus enhancing the overall output power
density.

4. Summary and Conclusions

In this work, a first step in modeling and simulating the thermal behavior of an
entire catalytic micro-monolith was performed. In particular, a CFD model was
developed for simulating three-channel and five-channel micro-combustors. For
both configurations, the operating maps were built as functions of the inlet gas
velocity, and compared to the operating map of a single-channel configuration.
Results show that, due to the relevant role played by heat losses in micro-
devices, it is not possible to extrapolate the behavior of the multi-channel
configurations from that of the single channel. Therefore, in order to predict
correctly performances and operating maps of catalytic micro-monoliths,
simulation of the entire reactor is needed. The main drawback of such an
approach is the computational cost. It has been found that the CPU time almost
linearly increases with the number of channels simulated.
The opportunity to feed the channels of the five-channel micro-combustor
with different mass flow rates was also investigated. It has been shown that, for a
fixed total mass flow rate, the global fuel conversion can be optimized by means
of a non-uniform distribution of inlet gas velocities among the channels.

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CFD of A Catalytic Micro-Monolith

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INTERNATIONAL JOURNAL OF CHEMICAL

National Research Council, dibenede@irc.cnr.it

National Research Council, disarli@irc.cnr.it

to the operating map of a single-channel configuration.

The conservation equations in the fluid are listed below (conventional

Fluent 6.3 (www.fluent.com). The

Table 1 Operating conditions for simulations

3. Results and Discussion

counterbalanced by the drawback of higher wall temperatures that are not

With configuration A, the homogeneous reaction front is stabilized inside

Kolaczkowski ST, Worth DJ. Modelling channel interactions in a non-adiabatic

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