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You are on page 1of 10

Amano

e-mail: amano@uwm.edu

Mohsen M. Abou-Ellail

e-mail: abouellail@hotmail.com

Mechanical Engineering Department,

University of Wisconsin-Milwaukee,

Milwaukee, WI 53201

S. Kaseb

Mechanical Engineering Department,

Cairo University,

Cairo 12613, Egypt

e-mail: kaseb@pathways.edu.eg

Numerical Predictions of

Hydrogen-Air Rectangular

Channel Flows Augmented by

Catalytic Surface Reactions

Catalytic combustion of hydrogen-air boundary layers involves the adsorption of hydro-

gen and oxygen into a platinum-coated surface, chemical reactions of the adsorbed spe-

cies, and the desorption of the resulting products. Re-adsorption of some produced gases

is also possible. This paper presents numerical computations of laminar momentum

transfer, heat transfer, and chemical reactions in rectangular channel ﬂows of hydrogen-

air mixtures. Chemical reactions are included in the gas phase as well as on the solid

platinum surfaces. In the gas phase, eight species are involved in 26 elementary reac-

tions. On the platinum hot surfaces, additional surface species are included, which are

involved in 16 additional surface chemical reactions. The platinum surface temperature

distribution is prespeciﬁed, while the properties of the reacting ﬂow are computed. The

results show very good agreement with the measured data. [DOI: 10.1115/1.4005202]

Keywords: catalyst, catalytic, channel ﬂow, surface reaction, hydrogen, platinum

1 Introduction

Platinum and palladium are common catalysts used to assist

combustion. The catalytic reactions can be beneﬁcial in porous

burners and catalytic reactors that use low equivalence ratios. In

this case the porous burner ﬂame can be stabilized at low tem-

peratures to prevent any substantial gas emissions, such as nitro-

gen oxides. Cattolica and Schefer [1,2] experimentally

investigated the combustion of hydrogen-air mixtures in bound-

ary layer ﬂows over catalytic and noncatalytic surfaces. In cata-

lytic combustion of hydrogen-air boundary layers, there involves

the adsorption of hydrogen and oxygen into a platinum-coated

surface, chemical reactions of the adsorbed species, and the de-

sorption of the resulting products. Re-adsorption of some pro-

duced gases is also possible. The catalytic reactions are found to

be very beneﬁcial in porous burners and catalytic reactors that

use low equivalence ratios. In this case the porous burner ﬂame

can be stabilized at low temperatures to prevent any substantial

gas emissions, such as nitrogen oxides. Combustion of several

fuels, i.e., NH

3

, CH

4

, C

3

H

8

and NH

3

/CH

4

mixture, on a platinum

surface in a stagnation ﬂow ﬁeld has been studied experimentally

by Williams et al. [3]. In addition, combustion of methane on a

platinum surface has been studied numerically by Song et al. [4].

In their work [4], the surface reactions of methane over platinum

have been modeled by a global reaction mechanism. Similarly,

combustion of hydrogen on a platinum surface in a stagnation

ﬂow ﬁeld and a boundary layer ﬂow ﬁeld has been studied

numerically by Warnatz et al. [5]. In their work, the elementary

reaction mechanism of the oxidation of hydrogen on a platinum

surface, including reactions of absorption/desorption of reactants

and products and reactions of surface radical recombination, has

been introduced. They also compared the computed [OH] con-

centration with experimental data from Cattolica and Schefer

[1,2]. However, Warnatz et al. [5] predicted values of OH one to

two orders of magnitude lower than those measured by Cattolica

and Schefer [1,2], at 1170 K surface temperature. Thermochemi-

cal data of surface species involved in the surface reactions have

also been published by Warnatz et al. [5]. Later, the elementary

surface reaction mechanism of methane with platinum has been

established by Deutschmann et al. [6]. The detailed surface reac-

tion mechanism has been used by Deutschmann et al. [6] to

numerically simulate the experiments of surface combustion of

methane over platinum conducted by Williams et al. [3]. It was

found that [6] methane is ignited at surface temperatures around

1000 K and the reaction is fast between surface temperatures of

1000 K and 1300 K; for surface temperatures below 1000 K, the

surface reaction is slow and the methane could not be ignited.

Surface coverage of surface species and mole fractions of gas-

phase species have been calculated by Deutschmann et al. [6] in

their work. Raja et al. [7] used the detailed surface mechanisms

for methane combustion [6] to model the catalytic honeycomb

monolith combustion.

In the present paper, the combustion of hydrogen-air mixtures

over catalytic surfaces is studied by numerical methods. The test

case, used to validate the present solution procedure, is that of a

reacting ﬂow of hydrogen-air mixture in a catalytic rectangular

channel. The test case ﬂow conﬁguration is shown in Fig. 1. A

parallel ﬂow of hydrogen-air mixture passes through the inlet sec-

tion of a rectangular channel coated with platinum. The equiva-

lence ratio of the hydrogen-air mixture is 0.32. The gas mixture

velocity at the channel inlet section is 1.6 m s

À1

while the gas tem-

perature is 313 K. A two-dimensional reacting ﬂow model, with

surface reactions, is developed for the rectangular channel geome-

try since the channel width is nearly 16 times its height. In this

case the ﬂow along the central section, perpendicular to the chan-

nel width, is two-dimensional in nature. A multistep reaction

mechanism is adopted for the gas-phase reactions. It involves 24

elementary reactions and 8 chemical species for hydrogen-air

mixtures. The multistep surface reaction mechanism is adopted

from the mechanism developed by Deutschmann et al. [6]. This

surface reaction mechanism consists of 16 elementary surface

reactions involving four gas-phase species and ﬁve surface spe-

cies. The surface reaction model developed by Coltrin et al. [8] is

adopted as a general layout for the present work. The present

Contributed by the Heat Transfer Division of ASME for publication in the

JOURNAL OF HEAT TRANSFER. Manuscript received October 29, 2010; ﬁnal manuscript

received September 24, 2011; published online February 13, 2012. Assoc. Editor:

Sujoy Kumar Saha.

Journal of Heat Transfer APRIL 2012, Vol. 134 / 041201-1 Copyright VC

2012 by ASME

Downloaded From: http://heattransfer.asmedigitalcollection.asme.org/ on 04/12/2013 Terms of Use: http://asme.org/terms

numerical predictions are compared with recent experiment and

numerical data.

2 Mathematical Model and Solution Procedure

The numerical model for laminar ﬂow, heat transfer, gas-

phase combustion, and catalytic surface reactions is presented.

The ﬂow conﬁguration investigated in the present paper is that

of a rectangular channel burner. Finite-volume equations are

obtained by formal integration over control volumes surround-

ing each grid node. Hybrid differencing is used to ensure that

the ﬁnite-difference coefﬁcients are always positive or equal to

zero to reﬂect the real effect of neighboring nodes on a typical

central node. The ﬁnite-volume equations of the reacting gas

ﬂow properties are solved by a combined iterative-marching

algorithm. On the platinum surfaces, surface species balance

equations, under steady-state conditions, are solved numeri-

cally. A nonuniform computational grid is used, concentrating

most of the nodes in the boundary sublayer adjoining the cata-

lytic surfaces. The ﬂow conﬁguration is shown in Fig. 1. The

numerical model can be classiﬁed into four main groups of

equations as follows.

2.1 Continuity and Momentum Equations. The mass conti-

nuity of the reacting ﬂow may be written as

@ðqÞ

@t

þ

@ðqu

i

Þ

@x

i

¼ 0 (1)

The momentum equation for the laminar reacting ﬂow may be

written in Cartesian tensor notations as [9]

@ qu

j

_ _

@t

þ

@

@x

i

qu

j

u

i

_ _

À

@

@x

i

l

@u

j

@x

i

_ _

¼ À

@ P ð Þ

@x

j

þ

@

@x

i

Â l

@u

i

@x

j

À

2

3

@u

k

@x

k

d

ij

_ _ _ _

(2)

where q is the gas density; u

j

is the gas velocity along coordinate

x

j

; l is the dynamic viscosity.

2.2 Energy Equations. The energy equation for the reacting

ﬂow is

@qh

g

@t

þ

@

@x

i

qu

i

h

g

_ _

À

@

@x

i

C

h

@h

g

@x

i

_ _

¼ À

j

DH

j

_ _

W

j

(3)

where h

g

is the gas sensible enthalpy; C

h

is the thermal diffusivity;

DH

j

and W

j

are the enthalpy of reaction and reaction rate of chem-

ical reaction j of the reaction mechanism involving hydrogen-air

mixtures; in the above equations, the subscript g denotes the gas

phase. The gas temperature at any point is directly related to the

local gas sensible enthalpy (h

g

), gas species mass fractions (Y

j

),

and constant-pressure speciﬁc heats, namely

h

g

¼

_

j

C

pj

Y

j

_ _

dT (4)

The lower limit of the above integration is 298 K, while the upper

limit equals the local gas temperature, T

g

.

2.3 Species Mass Fraction Equations. The species mass

fractions for the reacting channel ﬂow may be written as

@ðqY

l

Þ

@t

þ

@ qu

i

Y

l

ð Þ

@x

i

À

@

@x

i

C

Yl

@Y

l

@x

i

_ _

¼ M

l

m

lm

W

m

(5)

where Y

l

is the mass fraction of species l while C

Yl

is its molecular

diffusivity; M

l

is the molecular mass of species l;

lm

is the stoi-

chiometric coefﬁcient of species l in reaction m while W

m

is the

reaction rate of the elementary chemical reaction m of the present

reaction mechanism. It consists of 24 elementary reactions. The

present hydrogen-air chemical kinetic mechanism involves eight

species, namely, O

2

, O, OH, H, H

2

, H

2

O, H

2

O

2

, and HO

2

. The ele-

mentary reaction mechanism for hydrogen-air mixtures adopted in

the present work is the same as given by Tong et al. [10].

It should be mentioned here that

lm

is taken as a positive value

for products and negative for reactants as required for proper sum-

mation of the effect of each reaction on the net production of a

particular species.

2.4 Surface Reactions. For a steady-state problem, the solu-

tion has no change with respect to time. Thus, surface coverage of

any surface species with respect to time is zero. The variation of

the surface coverage with respect to time can be computed from

the net production of each surface species. The conservation of

the surface coverage of surface species k may be written as [5]

dz

k

dt

¼

_ s

k

Z

(6)

where z

k

is the surface coverage of surface species k, Z is the total

surface site density, and the surface density used in the present pa-

per is 1.63 Â10

15

cm

À2

[6]; _ s

k

is the net surface production rate,

in mol cm

À2

s

À1

, of the surface species k.

Since the present reacting ﬂow includes gas-surface interac-

tions, the mass transfer between the gas phase and the catalytic

surface needs to be included while solving the species mass frac-

tions of the gas species in the ﬂow. The mass ﬂuxes transferred

through the convection and the diffusion processes at the gas-

surface interface of any gas-phase species are balanced by the net

production or depletion rates of that species by surface reactions.

The surface boundary condition of each gas-phase species k based

on the mass balance is given by Coltrin et al. [8] as

n Á qY

k

V

k

þ u ð Þ ½ ¼ _ s

k

M

k

(7)

where n is the unit normal vector pointing outward with respect to

the surface, u is the bulk ﬂuid velocity, V

k

is the diffusion veloc-

ity, M

k

is the molecular weight of species k, _ s

k

is the net produc-

tion or depletion rates of gas-phase species k involved in surface

reactions.

The production rate of each species _ s

k

, either gas-phase species

or surface species, may be written as [11]

_ s

k

¼

Ks

j¼1

kj

k

fj

NgþNs

k¼1

X

k

½

0

k

j

(8)

where K

s

is the total number of elementary surface reactions;

0

kj

is left hand side stoichiometric coefﬁcients of the reaction

Fig. 1 Layout of the conﬁguration of reacting hydrogen-air

mixture ﬂow inside platinum-coated rectangular channel

041201-2 / Vol. 134, APRIL 2012 Transactions of the ASME

Downloaded From: http://heattransfer.asmedigitalcollection.asme.org/ on 04/12/2013 Terms of Use: http://asme.org/terms

equation; v

kj

is the right hand side minus left hand side stoichio-

metric coefﬁcients of the reaction equation; k

fj

is the forward ki-

netic rate constants; [X

k

] is the species concentrations; the units of

gas-phase species and surface species concentrations are mol

cm

À3

and mol cm

À2

, respectively; N

g

is the number of gas-phase

species while N

s

is the number of surface species.

A detailed surface reaction mechanism is used to model the

gas-surface interaction between the fuel and the platinum-coated

surface. The surface reaction mechanism adopted in the present

work, for hydrogen-air mixtures reacting over platinum-coated

surfaces, is established by Deutschmann et al. [6]. The surface

reaction mechanism consists of 16 elementary reactions and

involves four gas-phase species, namely, O

2

, OH, H

2

, H

2

O, and

ﬁve surface species, namely, O(s), OH(s), H(s), H

2

O(s), and Pt(s).

The reaction rate constants are described in terms of either the

Arrhenius expression or a sticking coefﬁcient, c. The Arrhenius

expression form is

k

fj

¼ A

j

exp

ÀE

j

RT

_ _

(9)

The sticking coefﬁcient can be converted to the usual kinetic rate

constants via the relation given by Coltrin et al. [8]

k

fj

¼

c

1 À c=2

1

Z

m

ﬃﬃﬃﬃﬃﬃﬃﬃﬃﬃ

RT

2pM

_

(10)

where Z is total surface site concentration, m is sum of the surface

reactants’ stoichiometric coefﬁcient, R is the universal gas con-

stant, T is the gas temperature at the catalytic surface, and M is the

molecular weight of the gas-phase species. The thermochemical

data needed to determine the rate coefﬁcients for the reverse reac-

tions and enthalpies of the surface species are provided by War-

natz et al. [5].

In the present work, steady-state conditions of the ﬂowing gas

and the surface species are assumed. Equations (6) and (8), in this

case, can be used to compute the surface species mole fractions,

given the gas species mole fractions at the interface between the

catalytic surface and the ﬂowing gas phase. Equations (7) and (8),

on the other hand, are used to compute gas species ﬂuxes at the

gas-surface interface. Although these ﬂuxes do not appear explic-

itly in Eq. (5), they are used to impose the proper boundary condi-

tions on the ﬂowing gas species ﬁnite-volume equations.

It should be mentioned here that the gas physical properties are

computed from temperature dependent relations. At any point in

the ﬂowing gas phase, the density is computed from the ideal gas

equation of state, while the viscosity is computed from a tempera-

ture polynomial of the third order. The species speciﬁc heats are

computed from temperature polynomials of the sixth order, which

are valid for 300 K to 2500 K temperature range [12]. The remain-

ing physical properties are deduced from the above properties and

Prandtl and Lewis numbers speciﬁed as 0.7 and 1.0, respectively,

for most gas species. However, the Lewis numbers of H

2

and H

are taken as 0.3 and 0.2, respectively, to reﬂect the faster diffusion

of these species with respect to the other heavier species such as

H

2

O and O

2

.

2.5 Numerical Solution Procedure. The two-dimensional

ﬂow inside the catalytic rectangular channel, shown in Fig. 1, is

overlaid with a ﬁnite grid of nodes. Equations (2), (3), and (5) and

the pressure correction counterpart of Eq. (1) are formally inte-

grated over the control volume surrounding each grid node. The

time dependent terms of the governing equations were dropped

out since the reacting ﬂow considered is under steady-state condi-

tions. The faces of the control volume bisect the distances

between the particular node and the four nearest neighbor nodes.

The formal integration is performed with due care to preserve the

physical meaning and overall balance of each dependent variable.

The ﬁnal form of the ﬁnite-volume equations are written as fol-

lows [9]:

a

n

ð Þ À S

P

_ _

W

p

¼

a

n

W

n

ð Þ þ S

u

(11)

where W stands for any of the dependent variables; namely, axial

and radial velocity components, gas sensible enthalpy, species

mass fractions, or the pressure correction which is used to satisfy

both mass continuity and momentum equations simultaneously.

The summation (R) is over the n four neighbors of a typical node

p. The above ﬁnite-difference coefﬁcients a

n

are computed using

the hybrid method, such that these coefﬁcients are always non-

negative to give the proper combined effects of convection and

diffusion. The above hybrid method is a combination of upwind

and central differencing schemes. Each scheme prevails for a par-

ticular range of the cell Peclet numbers, as given in detail by

Abou-Ellail et al. [9]. S

p

and S

u

are the coefﬁcients of the inte-

grated source terms at node p. The ﬂow in a rectangular channel

with dominant streamwise direction is parabolic in nature and

thus the hybrid scheme is accurate enough to eliminate any false

diffusion. In this case, the computational grid directions are

aligned along the main ﬂow direction and normal to it.

The solution procedure is based on the, line-by-line, tridiagonal

matrix algorithm (TDMA). The ﬁnite-volume equations (Eq. (11))

for each dependant variable are modiﬁed at the boundaries of the

solution domain, shown in Fig. 1, to impose the conditions there.

On the catalytic surface where y ¼0.0 mm, the velocity compo-

nents vanish while all other dependent variables’ normal gradients

reﬂect the mass and heat ﬂuxes due to surface reactions. Along

the axis of symmetry where y ¼3.5 mm and the exit section of the

ﬂow, the normal gradient is equal to zero. Moreover, for the cata-

lytic channel ﬂow, the transverse velocity is equal to zero at the

upper boundary where y ¼3.5 mm. At the inlet section, all varia-

bles are uniform. Within each computational loop of the gas

phase, Eq. (6) is solved, for all surface species concentrations,

iteratively at each transverse plane for steady-state conditions,

i.e., d(z

k

)/dt ¼0. The validation of the present numerical algo-

rithm is presented by Tong et al. [12] for heat and mass transfer in

impinging ﬂows on a hot catalytic surface. Tong et al. [12] com-

pared their results for temperature and species mole fractions in

the reacting impinging jet with numerical data of Deutschmann

et al. [6]. The agreement they obtained conﬁrms the accuracy of

the present numerical procedure [12]. Moreover, standard laminar

thermal boundary layer thickness and heat transfer data [13] were

also used for validation purposes by Tong et al. [14]. Further vali-

dation is given in the present work by comparing the present nu-

merical results with the experimental and numerical data of Appel

et al. [15].

3 Presentation and Discussion of Results

The catalytic surface reactions in channel ﬂows are investigated

numerically in this section. The numerical results are compared

with the recent experimental measurements conducted by Appel

et al. [15]. The rectangular channel, used by Appel et al. [15], has

its upper and lower plates coated with platinum. The height,

width, and length of the channel are equal, respectively, to 7 mm,

110 mm, and 300 mm. The ratio of width of the channel to the

height of the channel is large enough so that the ﬂow could be

considered two-dimensional in the vertical plane passing by the

centerline. The hydrogen-air mixture ﬂows through the channel

and reacts on the catalytic surface. The schematic plot of the chan-

nel ﬂow is shown in Fig. 1. The channel geometry shown in Fig.1

is used in the present numerical model. The grid used for the

channel ﬂow, namely the number of grid nodes along the x-axis

and y-axis is 10,000 and 330, respectively. Due to symmetry, only

the lower half of the computational plane, indicated in Fig. 1,

needs to be overlaid with the above grid of nodes. Moreover, the

axial increment Dx is taken as 3.0 Â10

À2

mm. The transverse grid

Journal of Heat Transfer APRIL 2012, Vol. 134 / 041201-3

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nodes are arranged such that 200 nodes lay inside the boundary

sublayer, i.e., in the range 0.0 <y <1.0 mm. The rest of the trans-

verse nodes lay outside the boundary sublayer, i.e., in the range

1.0 <y <3.5 mm. The above number of grid nodes is sufﬁcient to

handle the fast changing gas density and viscosity, both axially

and transversely inside the rectangular channel, as well as insuring

a grid-independent solution. With a total number of 3.3 million

grid nodes, it was necessary to utilize the parabolic nature of the

ﬂow. This is done through the use of a line-by-line TDMA scheme

to obtain numerical solutions in such a way to sweep the solution

domain from the inlet section to the exit section. The ﬁeld values

of the dependent variables are stored and then updated during the

subsequent iterations. The iterations are stopped when the ﬁnite-

volume equations of the dependent variables are satisﬁed with

errors less than 0.1%. This criterion is achieved with only three

iterations. The present numerical simulator is actually a combina-

tion of parabolic and elliptic procedures. It can thus be referred to

as a parabolic-elliptic procedure.

For the case being studied in the present work, the inlet velocity

of the gaseous mixture is 1.6 m/s, the inlet gas temperature is

313 K, and the equivalence ratio is 0.32. This case is referred to as

“case 2” in the experimental work of Appel et al. [15]. The surface

temperature proﬁle of the channel wall, along the x-axis was also

measured by Appel et al. [15]. Figure 2 shows the catalytic wall

temperature proﬁle along the streamwise direction. As shown in

Fig. 2, the surface wall temperature is not uniform. The wall tem-

perature at channel entrance is about 1060 K. It gradually

increases to a temperature around 1255 K then decreases to

1200 K near the channel exit section. This temperature proﬁle was

maintained by Appel et al. [15] with the help of guard heaters and

ceramic insulation. They also allowed the ﬁrst 60 mm of the chan-

nel to radiate to the cold surroundings to prevent the wall tempera-

ture from reaching super-adiabatic levels as a result of the faster

diffusion of the low- Lewis-number fuel, namely H

2

.

The curve ﬁtting equations that accurately describe the surface

temperature proﬁle (T

s

) are given below as

T

s

¼ 1062 þ 0:0089x

2:57

; 0 < x < 20 (12a)

T

s

¼ 1079 þ 1:80ðx À 20Þ

1:05

; 20 < x < 80 (12b)

T

s

¼ 1208 þ 3:20ðx À 80Þ

0:66

; 80 < x < 130 (12c)

T

s

¼ 1248:5 þ 0:23ðx À 130Þ

0:76

; 130 < x < 210 (12d)

T

s

¼ 1254:3 À 0:029ðx À 210Þ

2:02

; 210 < x < 265 (12e)

Equations (12a)–(12e) are used in the present work as the bound-

ary condition for the catalytic surface temperature axial proﬁle of

the channel ﬂow of Appel et al. [15]. Therefore, the heat gener-

ated by catalytic chemical reactions on the surface is not explicitly

considered in the present numerical computations. Figure 3 shows

the present numerical temperature transverse proﬁles together

with the experimental data of Appel et al. [15], at x ¼25, 85, 105,

165, and 235 mm. However, no experimental data for the 265-mm

section can be found. The present temperature proﬁles for the

measured ﬁve sections are in good agreement with the experimen-

tal data of Appel et al. [15]. Numerical computations were also

conducted by Appel et al. [15] using a fully elliptic computer

code that required 20,000 to 30,000 iterations depending on the

initial guess. They used 340 nodes along x-axis and 90 nodes

along the y-axis. They overpredicted the temperature of most of

the sections reported with a maximum error of 110 K between

their numerical and experimental data. However, as it can be seen

from Fig. 3, the experimental data of the gas temperature are well

predicted in the present work. This can probably be attributed to

the much ﬁner grid adopted in the present work. However, while

the present computer code uses a parabolic-elliptic solution proce-

dure that requires few iteration loops, Appel et al. [15] fully ellip-

tic procedure converged in 20,000 to 30,000 iterations depending

on the initial guess.

Figure 4 shows the mole fractions of H

2

and H

2

O at different

streamwise locations of 25, 85, 105, 165, and 235 mm. The mole

fraction of H

2

is multiplied by a factor of 2 for the purpose of

clarity. The predicted mole fraction streamwise proﬁles are com-

parable with the measured data of Appel at al. [15]. The stream-

wise mole fraction proﬁles of H

2

are in good agreement with the

experimental data up to a distance of 165 mm along the x-axis.

However, for x >165 mm, the H

2

mole fraction is slightly under-

predicted by the present solution procedure. Moreover, the nu-

merical results of Appel et al. [15] slightly underpredicted their

experimental data for all reported transverse planes, although

they used a costly fully elliptic numerical procedure. The pre-

dicted mole fraction transverse proﬁles of H

2

O are compared to

Fig. 2 Catalytic surface temperature proﬁle for the channel

ﬂow of Appel et al. [15]

Fig. 3 Transverse temperature proﬁles at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

041201-4 / Vol. 134, APRIL 2012 Transactions of the ASME

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the experimental data of Appel et al. [15], as depicted in Fig. 4.

The predicted mole fraction proﬁles of H

2

O are in good agree-

ment with the experimental data for the ﬁrst three transverse

planes. However, the numerical mole fraction proﬁles of H

2

O

overpredict the experimental data for the last two planes, as

shown in Fig. 4. This is an indication of an overprediction of the

H

2

O production rate that the adopted surface reaction mechanism

computes at the downstream locations where most of the plati-

num is inactive. Moreover, the numerical data of Appel et al.

[15] slightly overpredicted the experimental data for the last two

panes with x ¼165 and 235 mm. The difference in the level of

agreement between the present results and Appel et al. [15] pre-

dictions could hardly be attributed to the difference in the solu-

tion procedures. However, this better agreement is attributed to

the modiﬁcation in Eq. (10) that Appel et al. [15] adopted to

compute k

fj

in their numerical model. This modiﬁcation reduces

the speciﬁc reaction rate constants of the H

2

and O

2

adsorption

reactions at lower values of Pt(s) prevailing in the downstream

area of the inlet section.

In order to assess the merits of the present numerical work, the

ratio of the execution times of the present and Appel et al. [15] so-

lution procedures is thus estimated. The TDMA is used in the

present work and will be hypnotized as the solution scheme for

Appel et al. [15]. In the present work, TDMA is performed only

along the transverse direction and is repeated for all transverse

sections. However, for a fully elliptic solution procedure the

TDMA is normally applied along the streamwise (N

x

) and the

transverse (N

y

) directions. It should be mentioned here that N

x

and N

y

are the number of nodes along the x- and y-coordinates.

The ratio between the execution time of Appel et al. [15] and the

present work is estimated as the ratio between the two numbers of

iterations times the ratio between the two execution times per iter-

ation. The execution time of the TDMA(N

x

) together with the

execution time for computing the ﬁnite-difference equation coefﬁ-

cients is commonly assumed to vary with N

x

to an exponent hav-

ing a value between 1.0 and 2.0. If this exponent is taken as 1.5,

the estimated execution time of Appel et al. [15] is roughly 2

orders of magnitude higher than the present parabolic-elliptic so-

lution procedure execution time. As the TDMA algorithm is con-

sidered one of the most economical ﬁnite-difference equation

solvers, the above result should be taken as a nominal value rather

than an exact one.

The predicted oxygen mole fraction transverse proﬁles at differ-

ent streamwise locations are depicted in Fig. 5 for streamwise dis-

tances of 25 mm, 85 mm, 105 mm, 165 mm, 235 mm, and 265 mm.

The maximum value at each section occurs at the channel center-

line, as the oxygen is mostly consumed at the walls. At

x ¼265 mm, the proﬁles are completely ﬂat indicating the end of

most surface and gas reactions. Since the equivalence ration of

this ﬂow is 0.32, then residual oxygen is expected at the exit sec-

tion as can be seen from Fig. 5.

Figure 6 shows the transverse proﬁles of the streamwise veloc-

ity at distances along the x-axis of 25 mm, 85 mm, 105 mm,

165 mm, 235 mm, and 265 mm. The streamwise velocity shows

nearly a uniform proﬁle near the inlet section changing to a para-

bolic proﬁle near the exit section as it would be for ﬂow between

parallel plates. However, because of the excessive heating of the

gas mixture as it ﬂows along the channel axis, the centerline ve-

locity increases from 1.6 m/s at the inlet section to approximately

9 m/s at the exit section.

Figure 7 depicts the numerical transverse proﬁles of the trans-

verse velocity at streamwise sections of 25 mm, 85 mm, 105 mm,

165 mm, 235 mm, and 265 mm. The transverse velocity is highest

near the inlet section peaking to a value of about 2.2 cm s

1

.

Fig. 4 Mole fractions of H

2

and H

2

O at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 5 Mole fraction of O

2

at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

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Because of the symmetry of the channel ﬂow, the transverse ve-

locity is asymmetric with respect to the x-axis.

The OH mole fraction transverse proﬁles are shown in Fig. 8,

for streamwise distances of 25 mm, 85 mm, 105 mm, 165 mm,

235 mm, and 265 mm. For x <105 mm, the highest OH mole frac-

tions occur at the walls. However, at x ¼105 mm a peak for OH is

immerging which indicates the onset of a gas-phase ignition. The

peak OH value continues to increase at the subsequent sections

until it starts to decrease after x ¼235 mm.

Figure 9 shows the H mole fraction transverse proﬁles at differ-

ent streamwise sections. Near the inlet section the H mole fraction

is highest at the walls. However, a peak starts to appear away

from the wall for streamwise distances greater than 85 mm. This

peak increases with streamwise distances up to 165 mm where it

decreases with further increase in the streamwise distance. This

behavior is concurrent with that of OH. The O mole fraction trans-

verse proﬁles are depicted in Fig. 10 for streamwise distances of

25 mm, 85 mm, 105 mm, 165 mm, 235 mm, and 265 mm. Here the

trend of the O mole fraction proﬁles is similar to both mole frac-

tion proﬁles of OH and H. It is possible to conclude that a form of

high gas-phase reaction rates occur in the range of streamwise dis-

tances of 85 mm–105 mm. This could be attributed to local gas-

phase ignition.

The mole fraction transverse proﬁles of H

2

O

2

are depicted in

Fig. 11 for streamwise distances of 25 mm, 85 mm, 105 mm,

165 mm, 235 mm, and 265 mm. Near the inlet section, the H

2

O

2

Fig. 6 Streamwise velocity, u, at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 7 Transverse velocity, v, at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 8 Mole fraction of OH at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

041201-6 / Vol. 134, APRIL 2012 Transactions of the ASME

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mole fraction essentially vanishes. It starts to form two clear peaks

for x ranging from 85 mm to 165 mm. The H

2

O

2

mole fraction

proﬁles start to form one peak at the channel centerline for values

of x >165 mm where the temperature reaches its minimum value,

at each section. This behavior is dictated by two of the main ele-

mentary reactions that produce H

2

O

2

. These two reactions (R11

and R12f) increase with decreasing temperatures either because of

negative activation energy or negative temperature exponent [10].

Figure 12 shows the mole fraction transverse proﬁles of HO

2

for

streamwise distances of 25 mm, 85 mm, 105 mm, 165 mm,

235 mm, and 265 mm. Near the channel walls, two HO

2

peaks

start to form for streamwise distances of 85 mm, 105 mm, and

165 mm. They collapse into a central peak for streamwise distan-

ces in the range of 235 mm–265 mm. The production/consumption

rates of HO

2

are controlled by reactions R (5f) and R (5 b). The

ﬁrst reaction increases with decreasing gas temperatures while R

(5 b) is controlled by two temperature-conﬂicting-effect terms

[10].

Figure 13 depicts the streamwise proﬁles of the production rate

of H

2

O and consumption rates of H

2

and O

2

. It is interesting to

notice that the production rate of H

2

O is nearly equal to the con-

sumption rate of H

2

. Moreover, the consumption rate of H

2

is

nearly equal to twice the consumption rate of O

2

. This suggests

that the surface reactions can be summed up to a one step gas-

phase reaction as H

2

þ2 O

2

! H

2

O. In this case, the important

parameter would be the reaction rate in the above reaction. A cor-

relation for this reaction rate can be arrived at either experimen-

tally or from numerical data similar to the present data [12,14].

The H

2

O production rate decreases sharply in a short streamwise

distance of about 10 mm, as can be seen from Fig. 13. Figures 14

and 15 depict the surface coverage streamwise proﬁles of surface

species Pt(s), O(s), OH(s), H

2

O(s), and H(s). The surface platinum

Fig. 9 Mole fraction of H at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 10 Mole fraction of O at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 11 Mole fraction of H

2

O

2

at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Journal of Heat Transfer APRIL 2012, Vol. 134 / 041201-7

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decreases sharply from 1.0 to about 0.03 in a short distance of

about 5 mm; concurrently the O(s) surface coverage increases

sharply from 0.0 at the entrance to 0.97 at a streamwise distance

of about 5 mm, as can be seen from Fig. 14. Pt(s) then remains

nearly constant for most of the channel length, as can be seen

from Fig. 15. However, for x >150 mm the platinum surface cov-

erage gradually decreases to a value of 0.008. The reduction in the

platinum surface coverage implies that the adsorption reaction

rates must decrease. However, if the modiﬁcations in the surface

reaction rate constant equation were included in the present work

then these reaction rates would further decrease. The channel sur-

face remains mostly covered with O(s) for the remaining length of

the channel, as can be seen from Fig.15. Figure 15 depicts also the

surface overages of OH(s), H

2

O(s), and H(s). Along the channel

walls, the surface species OH(s), H

2

O(s), and H(s) increase

sharply from 0.0 to 4.0 Â10

À4

, 5.0 Â10

À8

, and 1.5 Â10

À8

,

Fig. 12 Mole fraction of HO

2

at streamwise distances of 25mm, 85mm, 105mm, 165mm, 235mm, and 265mm

Fig. 13 Surface production rate of H

2

O and Surface consumption rates of H

2

and O

2

Fig. 14 Surface coverage of surface species for 0<x<5 mm

041201-8 / Vol. 134, APRIL 2012 Transactions of the ASME

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respectively. These surface species continue to decrease along the

channel wall. At the channel exit section, the reductions in OH(s),

H

2

O(s), and H(s) are of orders of magnitudes ranging between

one and two. The streamwise pressure difference (p Àp

in

) proﬁle

is shown in Fig. 16. It is clear that the pressure decreases linearly

along the streamwise direction. The pressure difference stream-

wise gradient is approximately equal to À133 N m

À3

. This pres-

sure gradient could be useful in designing rectangular channel

catalytic burners.

4 Conclusions

The present parabolic-elliptic solution procedure is tested

against recent experimental and numerical data for reacting ﬂows

in catalytic rectangular channels. Through this study several con-

clusions emerged:

1. The agreement between the present results and the experi-

mental data is generally good and in some cases surpasses

the published numerical data for the same ﬂow. Moreover,

the present solution procedure is roughly two orders of mag-

nitude faster than the published fully elliptic numerical pro-

cedure for the same ﬂow conditions. The H

2

O is

overpredicted for sections near the exit section and is attrib-

uted to higher values of the adsorption reaction constants in

the downstream area, where the surface platinum is mainly

covered with O(s). The ﬁrst 0.7 L of the channel is vital in

building up the surface species and the depletion of the

active platinum sites. The numerical results show high pro-

duction rates of H

2

O in the vicinity of streamwise distance

of about 15 L.

2. The channel ﬂow computational results are compared with

recent detailed experimental data for similar geometry and

showed that the present numerical results for the gas temper-

ature, water vapor mole fraction, and hydrogen mole fraction

agree well with the experimental measurements, especially

in the ﬁrst 105 mm. However, some differences are observed

in the vicinity of the exit section of the rectangular channel.

The numerical results show that the production of water

vapor is very fast near the entrance section ﬂowed by a

much slower reaction rate. Gas-phase ignition is noticed

near the catalytic surface at a streamwise distance of about

120 mm. This gas-phase ignition manifests itself as a sudden

increase in the mole fractions of OH, H, and O.

Nomenclature

a

n

¼ ﬁnite-difference coefﬁcients due to combined convection

and diffusion, kg s

À1

Cp ¼ constant-pressure speciﬁc heat, J kg

À1

K

À1

DH

j

¼ enthalpy of reaction for reaction j, J mol

À1

h ¼ heat transfer coefﬁcient, W m

À2

K

À1

h

g

¼ gas sensible enthalpy, J kg

À1

k

c

¼ mass transfer coefﬁcient, kg m

À2

s

À1

L ¼ height of the computational domain, m

M ¼ molecular weight, kg kmol

À1

N ¼ number of grid nodes

Nu ¼ Nusselt number

P ¼ gas pressure, N m

À2

Pr ¼ Prandtl number

R ¼ universal gas constant, J mol

À1

K

À1

Re ¼ Reynolds number

R

s

¼ surface reaction rate, mol cm

À2

s

À1

_ s

k

¼ surface production or depletion rate of the surface species

k, mol cm

À2

s

À1

Sh ¼ Sherwood number

Fig. 15 Surface coverage of surface species for the total channel length (0<x >300mm)

Fig. 16 Streamwise pressure difference proﬁle (p-pin)

Journal of Heat Transfer APRIL 2012, Vol. 134 / 041201-9

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SPR ¼ surface production rate, mol cm

À2

s

À1

T ¼ temperature, K

u

i

¼ velocity in direction i, m s

À1

U

1

¼ uniform free stream axial velocity, m s

À1

W

j

¼ reaction rate of reaction j, mol cm

À3

s

À1

x ¼ streamwise distance, m

x

i

¼ distance along direction i, m (here, x ¼x

1

and y ¼x

2

)

X ¼ mole fraction

[X] ¼ generalized concentration (gas phase: mol cm

À3

, surface

phase: mol cm

À2

)

y ¼ transverse distance, m

Y ¼ species mass fraction

Z ¼ surface site concentration, mol cm

À2

z

k

¼ surface site fraction of k species (surface coverage

fraction)

Greek Symbols

d ¼ thermal boundary layer thickness, m

C

h

¼ thermal diffusivity, kg m

À1

s

À1

C

Yl

¼ molecular diffusivity of species l, kg m

À1

s

À1

l ¼ dynamic viscosity, kg m

À1

s

À1

q ¼ density, kg m

À3

c ¼ sticking coefﬁcient

Subscripts

g ¼ gas

s ¼ surface

x ¼ at a distance x from the inlet section

y ¼ distance from the wall

References

[1] Cattolica, R. J., and Schefer, R. W., 1982, “Effect of Surface Chemistry on the

Development of the (OH) in a Combustion Boundary Layer,” 19th Symposium

(International) on Combustion, The Combustion Institute, Pittsburgh, PA,

pp. 311–318.

[2] Cattolica, R. J., and Schefer, R. W., 1983, “Laser Fluorescence Measurements

of the OH Concentration in a Combustion Boundary Layer,” Combust. Sci.

Technol., 30, pp. 205–212.

[3] Williams, W. R., Stenzel, M. T., Song, X., and Schmidt, L. D., 1991,

“Bifurcation Behavior in Homogeneous-Heterogeneous Combustion: I. Experi-

mental Results Over Platinum,” Combust. Flame, 84, pp. 277–291.

[4] Song, X., Williams, W. R., Schmidt, L. D., and Aris, R., 1991, “Bifurcation

Behavior in Homogeneous-Heterogeneous Combustion: II. Computations for

Stagnation-Point Flow,” Combust. Flame, 84, pp. 292–311.

[5] Warnatz, J., Allendorf, M. D., Kee, R. J., and Coltrin, M. E., 1994, “A Model of

Elementary Chemistry and Fluid Mechanics in the Combustion of Hydrogen on

Platinum Surfaces,” Combust. Flame, 96, pp. 393–406.

[6] Deutschmann, O., Behrendt, F., and Warnatz, J., 1994, “Modeling and Simula-

tion of Heterogeneous Oxidation of Methane on a Platinum Foil,” Catal. Today,

21, pp. 461–470.

[7] Raja, L. L., Kee, R. J., Deutschmann, O., Warnatz, J., and Schmidt, L. D., 2000,

“Critical Evaluation of Navier-Stokes, Boundary-Layer, and Plug-Flow Models

of the Flow and Chemistry in a Catalytic-Combustion Monolith,” Catal. Today,

59, pp. 47–60.

[8] Coltrin, M. E., Kee, R. J., and Rupley, F. M., 1991, “Surface Chemkin: A Gen-

eral Formalism and Software for Analyzing Heterogeneous Chemical Kinetics

at a Gas-Surface Interface,” Int. J. Chem. Kinet., 23, pp. 1111–1128.

[9] Abou-Ellail, M. M., Gosman, A. D., Lockwood, F. C., and Megahed, I. E. A.,

1978, “Description and Validation of a Three-Dimensional Procedure for

Combustion Chamber Flows,” AIAA J. Energy, 2, pp. 71–80 (also, published in

Turbulent Combustion, L. Kennedy, ed., AIAA, New York, Vol. 58,

pp. 163–190).

[10] Tong, T. W., Abou-Ellail, M. M., Li, Y., and Beshay, K. R., 2004, “Numerical

Computation of Reacting Flow in Porous Burners with an Extended CH

4

—Air

Reaction Mechanism,” Proceedings of HTFED04, 2004 ASME Heat Transfer/

Fluids Engineering Summer Conference, Charlotte, NC, Paper No. HT-FED

2004-56012.

[11] Deutschmann, O., Maier, L. I., Riedel, U., Stroemman, A. H., and Dibble, R.

W., 2000, “Hydrogen Assisted Catalytic Combustion of Methane on Platinum,”

Catal. Today, 59, pp. 141–150.

[12] Tong, T. W., Abou-Ellail, M. M., and Li, Y., 2007, “Mathematical Modeling of

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Transfer, 21, pp. 512–519.

[13] Incropera, F. P., and DeWitt, D. P., 2001, Fundamentals of Heat and Mass

Transfer, 5th ed., Wiley, New York.

[14] Tong, T. W., Abou-Ellail, M. M., and Li, Y., 2007, “A Mathematical Model for

Heat and Mass Transfer in Methane-Air Boundary Layers With Catalytic Sur-

face Reactions,” ASME J. Heat Transfer, 129, pp. 939–950.

[15] Appel, C., Mantzaras, J., Schaeren, R., Bombach, R., Inauen, A., Kaeppeli, B.,

Hemmerling, B., and Stampanoni, A., 2002, “An Experimental and Numerical

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041201-10 / Vol. 134, APRIL 2012 Transactions of the ASME

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