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international journal of hydrogen energy 34 (2009) 64256436

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Numerical modelling and experimental validation


of a planar type pre-reformer in SOFC technology

Murat Peksen*, Roland Peters, Ludger Blum, Detlef Stolten


Institute of Energy Research-Fuel Cells (IEF-3), Forschungszentrum Julich GmbH, D-52425, Julich, Germany

article info abstract

Article history: A computational model of the Julich type pre-reformer and its experimental validation
Received 6 April 2009 used in solid oxide fuel cells (SOFCs) is introduced. A continuum modelling approach has
Received in revised form been attended and its feasibility verified. The fluid flow, heat transfer and chemical
8 June 2009 reacting species transport within the pre-reformer are numerically solved using 3D
Accepted 8 June 2009 computational fluid dynamics (CFD) based on the finite volume method. The model
Available online 2 July 2009 considers the typical sub-components of the pre-reformer including the solid frame, air
channels, catalyst and the wire mesh structures. Experimental measurements are used to
Keywords: supply appropriate boundary conditions for the simulations. The predicted results of the
CFD simulations are experimentally validated using thermocouples and gas chromatography.
SOFC The results show good agreement, implying that the proposed model is an invaluable tool
Pre-reformer that can be used to reduce costly experiments in the design and process optimisation of the
Methane-steam reforming pre-reformer.
Continuum model 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights
Conjugate heat transfer reserved.

1. Introduction Studies concerning SOFC modelling are mostly related to the


fuel cell stack, and the associated process parameters, rather
The solid oxide fuel cell (SOFC) technology presents great than the design and optimisation of individual SOFC system
economical and environmental potential for the next gener- components. Various researchers have focused on the reac-
ation power systems due to its energy efficiency and reduced tion kinetics, particularly of steam-methane reforming [415].
emission compared to the conventional power generation An extensive review of the general modelling techniques and
systems [1,2]. The SOFC operates at temperatures between articles comprising the fluid flow, heat transfer and electro-
600  C and 1000  C using hydrogen containing gases as the chemistry in planar type SOFCs is reviewed in detail by Col-
fuel. Hydrogen can be produced from a wide variety of pan et al. [16]. Ma [17] reviewed numerous articles concerning
resources, including renewable ones, nuclear energy and computational fluid dynamics modelling of fuel cells.
fossil fuels. There are about 90 hydrogen production routes Reviewed articles comprised many approaches ranging from
reported [3]. The major hydrogen source for SOFC systems 1D to 3D modelling. Recently, authors like Recknagle [18]
used for stationary applications is natural gas, particularly presented a 3D modelling of SOFC stacks.
consisting of methane. A detailed 3D simulation for an integrated SOFC stack is
The literature in the field of SOFC is mainly devoted to the also given by Haberman [19] investigating the stack perfor-
cell stack and the related physicochemical phenomena. mance based on process parameters. Boddu [20] introduced

* Corresponding author. Tel.: 49 2461 61 8732; fax: 49 2461 61 6695.


E-mail address: m.peksen@fz-juelich.de (M. Peksen).
0360-3199/$ see front matter 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijhydene.2009.06.017
6426 international journal of hydrogen energy 34 (2009) 64256436

Nomenclature Greek symbols


4 porosity,
c specific heat capacity, J/kg K
m viscosity, kg/m s
Dp mean particle diameter, m
r density, kg/m3
h enthalpy, J/kg
b inertial resistance coefficient,
k permeability, m2
p static pressure, Pa Abbreviations
T temperature, K CFD computational fluid dynamics
x, y, z cartesian coordinates, m SOFC solid oxide fuel cell
!u velocity magnitude m/s HCR heterogeneous chemical kinetics of reforming
!
u1 ; !
u2 and !
u3 components of the velocity GC gas chromatograph
magnitude, m/s
Subscript
f body force, N
f fluid
Dn porous layer thickness, m
s solid
keff effective thermal conductivity, W/mK
eff effective

a study on an alternative channel design for the fuel cell stack The plates with the air channels separate the air flow side
performance. Among a wide range of published research, from the fuel gas side to avoid any gas mixing. Hot air flows
however, little attention is shown to the design modelling of through the air channels, which is the main heating source of
SOFC components. For the total system development, cost the pre-reformer; therefore, the most important function of
and unscheduled outages, it is not sufficient to optimise the the air channels is to provide a uniform temperature distri-
fuel cell stack and then construct the plant around it [21]. The bution associated with the air flow. Two wire mesh structures
design, performance and allocation of each component play are placed between the air channel plates. The main purpose
a crucial role in the design of the entire multi-component of employing a wire mesh is to reduce the components
system, in order to maximise the desired output and reduce manufacturing effort by avoiding the use of a channel design
efficiency losses. on the fuel gas side. Hence, it should substitute the air chan-
At the Research Centre of Julich, a multi-component SOFC nels by distributing the fuel gas uniformly. The catalyst,
design based on planar stacks has been developed. The where the chemical reaction occurs, is sandwiched between
system components are integrated into a single package that the wire mesh structures.
enables the operation in self-sustaining mode. Details of the The pre-reformer operates such that hot air flows through
layout and the operation principle of the system were eluci- the air channels, by heating up the component. Using the
dated by Blum et al. [22]. To study and optimise the SOFC counter flow principle, methane containing fuel gas at speci-
system, it is necessary to investigate the effects of the design fied temperature and gas composition is released into the pre-
and operating parameters on the system components. In reformer. As the fuel gas gets in contact with the catalyst,
order to test the sensitivity of the parameters, one can reforming starts. During the chemically reacting species
perform a series of experiments with varying process transport of the fuel gas, methane is converted into H2 and CO,
parameters, construct prototype components, or develop and and the gas mixture enters the fuel cell with the desired
employ a model in an attempt to simulate the process and composition and temperature. Fig. 1 illustrates the typical
system behaviour of the components. Experimental component layout, and the counter flow operating principle of
measurements during the process of SOFC are prohibitive due the pre-reformer.
to the complexity of the processes and the design of the Numerical methods, such as the finite element or finite
components. To meet this challenge, computational model- volume method, enable modelling complicated geometry in
ling is becoming more sophisticated and the detailed a relatively short time while providing a solution sufficiently
descriptions of the flow, thermal, chemical and electro- accurate for engineering purposes. The numerical approaches
chemical processes have been increased in recent years. of computational fluid dynamics (CFD) have, in most cases,
One of the SOFC system components developed and tested proven to be a powerful tool to aid in reduced physical
at the Research Centre Julich is a special designed plate type prototype costs and product development time. In addition,
pre-reformer module using a plate type reformer catalyst. The they provide qualitative benefits such as the ability to consider
reformer is designed for both heated and adiabatic operation. more designs, efficiency gains, enhanced capacity, and the
It plays a major role in the SOFC system operation by heating availability of valuable information early in the process [23].
up the fuel gas to the fuel cell stack inlet temperature, and by There are many key parameters including the catalyst
reforming part of the fuel gas. This avoids excessive temper- type, operating conditions, reformer design features, and
ature gradients at the fuel cell stack inlet. Furthermore, it physical, chemical phenomena occurring in the reforming
converts the higher hydrocarbons that otherwise may lead to process that can influence the performance of the pre-former.
soot formation. The complete reformer consists of 10 stack Therefore, to acquire a better understanding of the pre-
units and includes four major sub-components, namely the reformer performance, and to improve the pre-reformer
air channels, wire mesh, the catalyst and the solid frame. A design, an extended knowledge of the processes, in particular
cover plate is also provided on top of the pre-reformer stack. the optimum fluid flow, heat transfer, chemical reactions
international journal of hydrogen energy 34 (2009) 64256436 6427

Fig. 1 Component layout and counter flow illustration of the pre-reformer.

along with the attendant species transport taking place within 2.1. Conservation of mass
the pre-reformer is required. Thus, without computational
fluid dynamics, detailed flow and heat transport characteris- The used equations are derived based on a continuum
tics essential to improving the pre-reformer design and approach, thus they are formulated in terms of the fluid
understanding of the pre-reforming process cannot be calcu- volume which is the porosity 4. The conservation of mass can
lated. Furthermore, it is possible to reduce the number of be expressed using the divergence operator as:
experimental tests by using CFD, since only a relatively small  
v frf   !
number of experiments are required to validate the accuracy V$ rf !
u V$ Ji fSm (1)
of the numerical results [24]. vt
In the present study, a 3D computational model of the where Sm refers to the rate of species produced due to the
!
planar type pre-reformer and its experimental validation is chemical reaction. Ji is the mass diffusion flux of species i.
introduced. The model considers the typical sub-components Equations solved within the gas channels consider the
of the pre-reformer including the air channels, solid frame, porosity as unity.
catalyst and the wire mesh structures. A continuum model-
ling approach based on the porous media theory is tested, and
its feasibility verified using micro modelling of the wire mesh 2.2. Momentum equation
structure. Various material properties and process parameters
used in the modelling approach are supplied from the To describe the flow behaviour of the pre-reformer, in addi-
measurements performed in Julich. In order to validate the tion to the standard field equations, constitutive equations are
predicted CFD results, thermocouples located in the solid needed. In the solution of the momentum equation, the
frame of the reformer, and a micro gas chromatograph is used porous media is modelled by the addition of a momentum
to determine the temperature distribution of the pre-reformer source term to the NavierStokes equations. The source term
and the gas composition of the species respectively. existing due to the porosity of the medium has been essen-
tially described by Darcys Law and is well established for flow
through porous media [2628]. Air permeability measurement
2. Mathematical modelling results obtained from previous studies showed clearly that the
flow through the used wire mesh structure is non-linear [29].
In order to make detailed and accurate predictions of the This proposes that the flow through the investigated
planar type SOFC pre-reformer with air and fuel gas supply, reformer system comprises not only the effect of viscous
several physicochemical processes have to be modelled. The resistance in terms of Darcys law, but is also characterised
mathematical formulation of the thermo fluid flow through macroscopically considering the effect of inertia on flow
the pre-reformer accompanied with species transport and through the porous layers. The non-linear Forchheimer term
chemical reaction is given in this section. The 3D non-linear [30], describing the kinetic effect of the fluid, is included to the
equations are applied such that the physical values of the NavierStokes equations. The departure of measurement
reformer sub-layers are locally averaged over a representative results from the predictions calculated by Darcys law is due to
elementary volume [25]. this term.
6428 international journal of hydrogen energy 34 (2009) 64256436

The used source term in the modelling approach is Yi in Eq. (6) is the mass fraction of species i, and the partial
composed of two parts: a viscous loss term and an inertial loss enthaply hi of the i-th species is formulated as:
term: Z T
 
m brf ! ! hi Cpi TdT hfi (7)
Si  juj u (2) Tref
k 2
hfi denotes the specific enthalpy of formation of the species in
This momentum sink Si contributes to the pressure gradient
the fluid mixture at Tref . Any enthalpy change due to chemical
in the porous cell, creating a pressure drop for a specified
reaction is included to the energy conservation because of this
thickness of the porous layer. The first part of the right-hand
term. Tref is assumed to be as 298.15 K. The effective thermal
side of Eq. (2) describes the viscous loss term where k is the
conductivity keff is calculated using the continuum theory of
fluid permeability, m the dynamic viscosity, and ! u the velocity
mixtures considering the volume fraction of solid and fluid
vector. The reciprocal value of k is the constant viscous
regions, and can be expressed as:
resistance factor. The Forchheimer regime is presented as
inertial effects, in the second term of the momentum source. keff fkf 1  ffks (8)
b and rf present the inertial resistance coefficient and the fluid
density, respectively. Details of how to derive the constants The mass diffusion flux of the species is due to the thermal
are elucidated by Peksen et al. [31]. and species concentration gradients. Diffusion of pore level is
Hence the momentum equation describing the system is neglected, and the mass diffusion is described using macro-
expressed as: scopic equations for isotropic, continuous media. To calculate
the mass diffusion within the pre-reformer, a non-dilute
 
vf!u m brf ! ! mixture in laminar flow approach is considered. The Maxwell
rf rf f!
u $V!
u fVP mV2 f!
u juj u (3)
vt k 2 Stefan equation for multi-component species transport is
In order to present the viscous and inertial loss coefficients employed. The mass diffusive flux is calculated as:
in the air channels, a correction factor of 0.8892 is used [32] to
! X
N1
VT
present the rectangular shape. Ji  rDij VYj  DT;i (9)
j1
T

2.3. Energy equation Dij is the binary mass diffusion coefficient of component i in
component j. Yj refers to the mass fraction of species j. The
The energy equation for the porous area and the solid region thermal diffusion coefficient of constituent i is denoted as DT;i .
(the wall of the pre-reformer) is differently solved. In porous Merk [33] showed that by assuming same external forces on
media regions, the energy conservation equation is solved all components, and by neglecting the pressure diffusion, the
with modifications to the heat conduction flux and the tran- diffusion coefficients for binary systems are the same as the
sient terms. The heat conduction flux uses an effective diffusion coefficients for a multi-component system. This
thermal conductivity and the transient term includes the result is adopted to employ the binary diffusion coefficients in
thermal inertia of the solid region on the medium. In the solid the multi-component system. The mass diffusion coefficients
regions, specific energy is conserved, internal heat generation in the mixture are expressed as:
is omitted, and the pressure terms drop. The general form of
the energy equation for the coupled conjugate heat transfer 1  Xi
Di;m P  X  (10)
problem can be expressed as follows: j
Dij
j;jsi
v    
frf Ef 1  frs Es V$ ! u rf Ef p The physical and chemical properties of the gas species are
vt
" ! # crucial for the mixture gases, particular for the reacting gases.
X !
V$ keff DT  hi Ji s$ u Se (4) For the SOFC applications, the gas mixtures can be assumed as
i
ideal gases due to the high temperatures and low pressures
where Ef is the total fluid energy, Es, the total solid region that occur during processing. The thermophysical properties
energy, f the porosity of the medium. keff, refers to the of the used gases are defined by comparing the studies of
effective thermal conductivity of the medium, and Se is the Knacke et al. [34], Todd and Young [21], and Kostka [35].
!
fluid enthalpy source term. The term Ji is the mass diffusion
flux of species i. The first three terms on the right-hand side of 2.4. Chemical reaction
Eq. (4) represent energy transfer due to heat conduction,
species diffusion, and viscous dissipation, respectively. Experiments performed by Drescher [36] showed clearly that
The total energy E of the components, i.e. fluid or solid for the employed catalyst and temperature range, two major
region is in Eq. (4) defined as: chemical reactions occur during the methane reformation.
Thus, the reaction scheme for the present study covers the
p u2
Eh (5) methane-steam reforming, expressed as:
r 2

where sensible enthalpy h is defined for incompressible flows CH4 H2 O%CO 3H2 DRH0298 K 206 kJ=mol (11)
as
X and the water-gas shift reaction, defined as:
p
h Yi hi (6)
i
r CO H2 O%CO2 H2 DRH0298 K 41:2 kJ=mol (12)
international journal of hydrogen energy 34 (2009) 64256436 6429

It should be noted that the reforming reaction is endo- 1


r CH4 H2 O  COH2 3 (16)
thermic and the overall reaction balance needs heat to kx
proceed. The required heat is provided by the air flow through where kx can be expressed as:
the channels, which are also modelled, rather than applying
a constant heat flux, or constant temperature on the bound- XN
  00 0
aries. Experiments performed at steam to carbon ratios above hfi TDS0 P i 1 ni r  ni r

1.6 and within the temperature range the pre-reformer oper- kx e RT RT (17)
ates, showed that a carbon deposition is negligible low; hence
With an equilibrium constant described in terms of partial
the use of a multi step heteregenous reaction kinetics
pressures of the species, and converting the present expres-
considering the carbon coverage is not required. Hofmann
sion in an Arrhenius form yields to:
et al. [37] compares a global kinetic approach with the HCR
 
method, considering the reforming behaviour of methane, PCO P3H2 Ea
and the solid region temperature profiles. Discrepancies of r kr PCH4 PH2 O  e RT (18)
kp p20
methane conversion rates and flatter temperature profiles are
Using the equation of state for ideal gases, all the pressures
elucidated, obtained by the used HCR method. Sensitivity
are then expressed in terms of concentration. Measurements
analyses are performed to predict similar results as the global
of the anode gas composition showed clearly that the CO gas
kinetic approach. In fact, the choice of the model employed
concentration within the investigated temperature range was
should be based on experimental investigations. Considering
higher than the calculated values for the thermodynamic
the in-house measured temperature profiles and methane
equilibrium composition [12]. This suggests that the shift
conversion rates, a differential rate law relating the rate of
reaction is not in equilibrium; therefore, the kinetic plays also
reaction to the rate of change in concentrations of the species
a rate limiting role during the water-gas shift reaction, thus
is used. Generally the chemical reaction kinetics can be
a similar model was used to consider the kinetic limiting role
expressed as:
of the water-gas shift reaction as well. The required parame-
ters such as the pre-exponential factor kr and the activation
Y
NR Y
NR
ri kf Cj h0  kb Cj h00 (13) energy Ea defined in the Arrhenius equation are determined
j1 j1 from the experimental data performed on an anode cermet
Where NR is the number of the chemical species in the reac- consisting of Ni-8YSZ substrate with a standard composition
tion, Cj the molar concentration of each reactant and product, of 50 % Ni [12]. Results of the data fit using a Levensberg
h0 is the forward rate exponent of each reactant and product Marquardt algorithm provided the required input data used in
species, and h00 is the backward rate exponent. According to the numerical calculations. Further assessment of the physics
the general description, the reforming rate can be described and parameters considered in the study are in progress.
as:

r kf CH4 H2 O  kb COH2 3 (14)


3. Computational modelling
kb
r CH4 H2 O  COH2 3 (15) The mathematical model for the solution of the fluid flow,
kf
heat transfer and chemically reacting species transport is
The equilibrium constants kf (forward) and kb (backward) solved using computational fluid dynamics, based on a finite
can be expressed as a concentration equilibrium constant kx, volume approximation. CFD analyses have to be very carefully
so that the reaction kinetics are only functions of the forward planned and executed, which will contribute significantly to
reaction. This yields to the reaction: the success of the modelling effort; therefore, in this section,

Fig. 2 Temperature contour plot results of (a) discrete approach and (b) continuum approach.
6430 international journal of hydrogen energy 34 (2009) 64256436

Fig. 3 Pressure contour plot results of (a) discrete approach and (b) continuum approach.

a 3D feasibility study of the continuum approach compared to occurring with reduced material properties for the solid and
a discrete approach is introduced. fluid phases can be treated with the mixture theory, because
the individual parts of the mixture cover the total control
3.1. Feasibility study space [31]. The analysis of the complex woven structure of the
wire mesh will not only provide an understanding of the
A thorough understanding of the pre-reformer requires complex geometry, but will give an insight in interpreting the
a careful modelling strategy. The wire mesh structures sand- results for showing the limits of a continuum model
wiching the catalyst is the sub-component showing the most compared to a discrete model. Furthermore, the feasibility of
complicated geometry within the pre-reformer, due to its a continuum approach will also ensure that the CFD analyses
wavy structure. This increases the computational effort remain in the frame of the allocated computational memory.
tremendously. To exploit its geometrical exact affect on the The woven structure is characterised by the orthogonal
pre-reformer performance, a continuum modelling approach interlacing of two sets of metal threads running perpendicular
is verified using the discrete model of the wire mesh repre- to the direction of the other. Where, each thread is undulated
senting its micro geometry. The idea is to replace the micro and passes over or under another thread. A conjugate heat
geometry with a hypothetical homogeneous macro one, transfer analysis using the CFD technique is performed. The
which considers the distributed mass of the solid body and the thermo fluid flow behaviour of the wire mesh without chem-
fluid over the total control space. The distribution is achieved ically reacting flow is investigated to understand the differ-
using the porosity of the continua. The substitute continua ences between the attended two approaches. The benefit of

Fig. 4 Computational model of the pre-reformer: (a) discrete and continuum model of the pre-reformer; and (b) symmetrical
CFD model using the continuum approach.
international journal of hydrogen energy 34 (2009) 64256436 6431

Fig. 5 Pre-reformer stack, and the specified thermocouple locations on the plate.

a conjugate analysis compared to an isothermal analysis is, illustrated in the surface plane shows very good agreement.
that it enables solving within the solid region simultaneously Thermal gradients within the wire mesh are not visible, which
with the fluid flow, thus the temperature distribution within is expected due to the large thermal conductivity differences
the structure can be thoroughly investigated. between the solid region and the fluid domain. The wire mesh
material is more conductive than the fluid thermal conduc-
3.1.1. Temperature field analysis tivity, which results in a uniform temperature distribution
Fig. 2 shows the temperature contour plot results of the 3D within the metal threads. The thermal resistance remains
wire mesh structure obtained from the discrete model anal- exclusively outside the thread.
ysis, and the continuum modelling approach with the same
constituents dimensions including the wire diameter, 3.1.2. Pressure field analysis
porosity and position in the computational fluid domain. The Fig. 3 illustrates the pressure contour plots of the performed
continuum model required over 44,000 cells, whereas the analyses. The continuum model includes the experimentally
discrete model occupied over 77,000 cells. The same boundary determined pressure drop of the wire mesh. Pressure values
conditions are applied in both approaches. The inlet and present the gauge pressure values, thus the negative values.
outlet distances are set to the exact positions within the fluid Due to the wavy structure, the wire mesh is subjected to
domain. Hence the results are on the same scale to perform an drag reduction and fluctuating lift coefficients. The pressure is
exact comparison. positive upstream whereas it becomes negative downstream
The contour plots illustrate the wire mesh structure and from the wavy surface. The predicted results of the
a surface plane of the fluid domain passing through the wire continuum approach are in very good agreement with the
mesh. The temperature profile of the predicted results reveals discrete approach providing the same pressure distribution.
that in steady state the temperature value of the wire mesh The pressure difference in the upstream and downstream
reaches the same value in both approaches. Furthermore, the regions on each side of the threads is accurately captured by
comparison of the developing temperature profile of the fluid the continuum approach. The results of both the thermal

Fig. 6 Gas chromatograph facility used to determine the fuel gas composition.
6432 international journal of hydrogen energy 34 (2009) 64256436

material properties. Performing a 3D analysis in design


Table 1 Process conditions for pre-reformer stack.
purposes is essential, hence a 2D approach which was tested
H2O/CH4 T_Air T_Fuel Air_Mass Fuel_Mass is not considered in this study. The modelled pre-reformer
[ C] [ C] flow rate flow rate
shows both flow and geometrical symmetry; therefore, to fit
[kg/h] [kg/h]
the problem within the memory constraints of the computer,
Case_A 2.4 723 155 30 2.55 half section of the system is considered. Fig. 4 illustrates the
Case_B 2.5 699 154 15 2.56 discretely modelled pre-reformer and the substitute
Case_C 2.5 641 153 7 2.57
continuum model (a), and the CFD model together with the
applied boundary conditions and sub-components (b).
The fluid inlet regions for air and fuel gases are specified as
behaviour and the pressure distribution show that the use of mass flow rates and temperatures together with species
the continuum modelling approach is feasible and provides concentrations that are provided from experimental data.
sufficient accurate results to be employed in the CFD analysis Considering the low fluid flow velocities associated with low
of the pre-reformer component. Moreover the discrete model Reynolds numbers enables the physical modelling approach
requires approximately twice more cells as it is the case for as to be laminar flow. The analyses are performed in steady
the continuum model. It should be noted that a much coarser state combined with heat transfer, species transport and
mesh can be used for the continuum model investigated, chemical reaction. The model may also be used in transient
whereas due to the wavy structure this cannot be performed simulations. No-slip conditions are applied at wall boundaries
for the discrete model. The difference of cell number used will (u v w 0). Zero heat flux is specified on top and bottom of
increase when the whole wire mesh would be considered, the model. The fluid mixtures within each modelling zone are
because the cell size difference between the employed cells considered to be incompressible-ideal gases, i.e. for air heat-
should not be too much to avoid numerical errors; therefore, ing and the fuel gas. The calculation of the pressure value is
the tiny cells used in the discrete geometry must be compat- achieved from the continuity equation. For this purpose
ible with the fluid domain around it, thus the cell number a velocity pressure coupling is applied using the SIMPLE
increases. The continuum model has no complicated geom- (Semi-Implicit Pressure Linked Equations) algorithm. For
etry; therefore, the grid size can be much more tolerable, details of the method, refer to Veersteg and Malalasekera [38].
which enables the use of less cells. Hence the computational The numerical accuracy is assessed by investigating the grid
modelling of the pre-reformer is carried out using the resolution and criteria for iterative calculations. Furthermore,
continuum modelling approach. the solution is validated using experimental measurements.

3.2. Continuum modelling using 3D CFD

The 3D continuum model is developed to substitute the 4. Experimental measurements


discrete model. It includes the typical sub-components of the
pre-reformer system, i.e., the air channels, wire mesh struc- 4.1. Reformer surface temperature measurements
tures, solid frame and the catalyst. Apart of the solid frame,
each component of the system is treated as a porous zone, To characterise the thermal behaviour of the pre-reformer,
which is modelled as a continuum phase considering effective the temperature distribution is an important parameter. The

Fig. 7 CFD simulations and experimental validation: (a) pre-reformer temperature distribution; and (b) fuel gas species
composition.
international journal of hydrogen energy 34 (2009) 64256436 6433

Fig. 8 Temperature and methane distribution along the catalyst: (a) Case_A; (b) Case_B and (c) Case_C.

reforming rate is set by the reformer operating temperature, using K type thermocouples, which are housed well into the
controlled by the amount of hot gas released into the reformer frame. This permits real surface contact whilst
reformer. The reformer air inlet is fed directly with the SOFC attached to the solid wall. The temperature of the reformer is
stack cathode outlet gas. Therefore, the air inlet temperature measured at specified locations, enabling a distribution along
of the reformer is determined by the SOFC operation. The the plate (Fig. 5). The results of the measurements will be used
chemical reaction kinetics is temperature dependant and for the validation of the numerically predicted computational
governs the maximum methane conversion rate that is ach- fluid dynamics (CFD) analyses.
ieved when chemical equilibrium is reached within the fuel
gas region. Therefore, controlling the reformer temperature 4.2. Fuel gas composition measurements
ensures the desired catalyst temperature that is associated
with the reformer performance. To measure the surface To determine the fuel gas composition at the entrance and
temperature of the pre-reformer, experiments are conducted exit of the pre-reformer, a micro gas chromatograph (GC)
6434 international journal of hydrogen energy 34 (2009) 64256436

Fig. 9 Velocity distribution and pathlines along the wire mesh layer and manifolds: (a) Case_A; (b) Case_B and (c) Case_C.

produced by Varian, Inc. is used. The gas mixture is dried temperature profiles also imply that the process is sensitive to
before being sent to the GC. Argon is used as the carrier gas. pressure, as expected. Higher partial pressures (associated
Both steam and argon cannot be detected; therefore, the with mole fractions) not only enhance the forward reactions,
measured results are assumed to be balanced by argon. but also the backward reactions. Thus, higher temperatures
The inlet gas composition is determined at the beginning of leading to lower methane and steam partial pressures result
the test sequence, whereas the gas composition values at the at the same time in higher partial pressures of the reaction
outlet are resolved after the process has reached steady state. products. Fig. 8 illustrates the detailed temperature distribu-
A complete analysis is achieved without using conventional tion and methane mass fraction results of the fuel gas over the
multi-column or multi-valves. Fig. 6 illustrates the gas chro- catalyst.
matograph facility. The presented results show that higher process temperatures
lead to higher thermal gradients within the catalyst (Case_A),
4.3. CFD results and experimental validation whereas these reduce when low temperatures are applied
(Case_C). The conjugate heat transfer resulting from the air
The proposed 3D model is validated using the pre-reformer channels to the wire mesh and catalyst leads to hotter zones at
surface temperature measurements and species gas compo- the vicinity of the air channel inlet side, whereas the cooler zones
sitions. CFD simulations were performed for three different are due to the colder convective fuel gas flow, which the catalyst
cases presented as A, B and C. The inlet process conditions for is directly subjected to. The methane mass fraction distribution
the simulated sets are given in Table 1. clearly demonstrates the fact that due to higher temperatures,
Fig. 7 illustrates the temperature distribution (a) and the less methane is retaining at the outlet region, thus more heat is
fuel gas outlet composition (b) of the pre-reformer together absorbed from the pre-reformer. The main purpose of the wire
with the experimentally determined values. Measurement mesh layer is to provide a uniform flow distribution. Therefore, it
results present the solid body temperature. is important to get a better understanding of the flow behaviour of
The temperature distribution curve of the pre-reformer the wire mesh. Fig. 9 illustrates the velocity distribution results
shows at high temperatures a steeper behaviour, and tends to for the three sample cases.
be declining at low temperature ranges. This is attributed to The predicted results show that the fuel gas flows uniformly
the high methane conversion rates at high temperatures (59%) through the wire mesh structure as it is desired. The different
and the associated rate constants. The species mole fraction contour values of each case are due to the different mass flow
bars indicate that operating at high temperatures leads to rates, which are expected. As the thermo fluid flow through the
reversed reaction rates according to the Arrhenius equation, air channels is the main heating source of the pre-reformer,
and the carbon concentration will decrease as a result. The particular importance is given to the flow behaviour of the air

Fig. 10 Velocity distribution and pathlines along the air channels and manifolds: (a) Case_A; (b) Case_B and (c) Case_C.
international journal of hydrogen energy 34 (2009) 64256436 6435

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