Integrated HT-PEMFC and Multi-Fuel Reformer For Micro CHP

Integrated HT-PEMFC and multi-fuel reformer
for micro CHP
Program theme: Fuel Cells

ForskEL ID: 010104
Final report
Table of Contents
List of Figures..................................................................................................................... i
Project summary .............................................................................................................................. 2
Introduction...................................................................................................................................... 3
WP 1: Detailed characterization of HT-PEMFC ................................................................................ 3
Application of EIS to cell and stack characterization ................................................................... 3
Development of in-situ sensors ................................................................................................... 7
Durability studies ......................................................................................................................... 9
WP 2: Development of multi-fuel reformer................................................................................... 10
WP 2.1 Characterization and modeling of catalyst .................................................................... 10
WP 2.2 Development of 2nd generation optimized multi-fuel reformer ................................... 14
Flue gas side ............................................................................................................................... 15
Reformate side ........................................................................................................................... 16
FEM analysis ............................................................................................................................... 19
Reformer testing ........................................................................................................................ 20
Conclusions on WP2.2 ................................................................................................................ 22
AP 3: Development of integrated micro CHP system .................................................................... 23
Development .............................................................................................................................. 23
Tests ........................................................................................................................................... 24
Conclusions from AP 3 ............................................................................................................... 24
Communication of project results.................................................................................................. 24
List of enclosed material ................................................................................................................ 25
Enclosure A .........................................................................................................................................
Enclosure B .........................................................................................................................................
Enclosure C .........................................................................................................................................
Enclosure D.........................................................................................................................................
Enclosure E .........................................................................................................................................
Published Papers ................................................................................................................................

Integrated HT-PEMFC and multi-fuel reformer for micro CHP
PSO2008 ForskEL ID: 010104
List of Figures
Figure 1: Single cell test setup applied for Electrochemical Impedance Spectroscopy
measurements. .................................................................................................................................... 4
Figure 2: Overall testing procedure applied in the LabView based EIS system. .................................. 4
Figure 3: (left) illustration of a Nyquist plot of EIS data and a related equivalent circuit model
(right) relation between cell components / losses and the equivalent circuit.................................... 5
Figure 4: Nyquist plot of EIS data collected on a single cell at different temperatures. ..................... 5
Figure 5: Charge transfer resistance as function of temperature derived from equivalent circuit
model. .................................................................................................................................................. 6
Figure 6: Gas transfer resistance as function of cathode stoichiometry. ............................................ 6
Figure 7: Nyquist plot of EIS measurements at four temperatures conducted at stack level............. 7
Figure 8: Schematic of thermocouples inserted in the bipolar plates on the cathode (left) and
anode (right) sides of the operating fuel cell....................................................................................... 8
Figure 9: (left) cathode and anode flow rates versus time (right) resulting temperatures recorded
locally on the MEA. .............................................................................................................................. 8
Figure 10: (left) Interior of container used for long term stack tests (right) Hydrogen supply system
with automatic changeover between hydrogen batteries. ................................................................. 9
Figure 11: End-of-life cell potential after 40.000 hours as function of operating temperature and
CO concentration in the hydrogen feed. ........................................................................................... 10
Figure 12: FT-IR gas analyzer (left) and mass spectrometer (right). .................................................. 11
Figure 13: FLS-Airloq gas analyzer...................................................................................................... 12
Figure 14: Photo of the catalyst test facility with main components labelled. ................................. 13
Figure 15: LabView interface for data acquisition and control of the test facility. ........................... 13
Figure 16: Illustration of region with flue gas bypass. ....................................................................... 15
Figure 17: Illustration of flue gas bypassing the cassettes (red areas corresponding to high gas
velocity) leading to poor heat transfer to the reforming reaction consequently low conversion.... 16
Figure 18: Test setup used for pressure distribution tests on a single cassette................................ 17
Figure 19: Calculated flow distribution around wiremesh at different values of and . ............... 17
Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Final report
Figure 20: Outline of the CFD model with the flow in U-configuration. ............................................ 18
Figure 21: Predicted flow distribution between cassettes in the reformer for U- and Z-
configurations. ................................................................................................................................... 19
Figure 22: Predicted flow distribution with a 3 fold increase in manifold diameter for the U- and Z-
configurations. ................................................................................................................................... 19
Figure 23 System performance of test system, fuelled on methane and biogas .............................. 21
Figure 24 Methane slip and catalyst temperature of test system fuelled on methane and biogas.. 21
Figure 25 Temperature profile in the reformer ................................................................................. 22

Final report
Project summary
The project was initiated in April 2008 and completed by the end of March 2010. The project
consortium consisted of: Dantherm Power, Serenergy and Department of Energy Technology at
Aalborg University (project manager). The activities were coordinated with the project Nordjysk
H2FC Center funded by the Region of Northern Jutland.
A number of experimental characterization methods were developed through this project to

improve the understanding in fuel cell performance under different operating conditions. In
particular the application of Electrochemical Impedance Spectroscopy was found useful and lead
to new information about individual losses in the fuel cell. Techniques to measure local
temperatures of the MEA were also successfully developed.
Durability studies were made on single cells as well as complete stacks. A dedicated test facility
was constructed in a container to isolate the test from disturbances that occur in the laboratory.
The stack tests were run for just above 6 months with few interruptions and it was found that
single cell and stack degradation rates were comparable. Operation temperature was found to
have the most pronounced influence on degradation. The information formed the basis for a
simple modeling tool to optimize the stack operating temperature versus reformate gas CO
concentration.
The activities on multi-fuel reformer development were mostly focused on two issues;
manufacturability and analyses of flow distribution and heat transfer. The latter was required
since these areas these turned out to cause challenges in the reactor design. Through a
combination of experimental tests, CFD analyses and flow network modeling design modifications
were suggested to improve flow distribution on both the flue gas side and the reformate side.
Most of these design changes were not validated in this project through the construction and test
of a new reformer. In spite of the problems identifies, the reformed successfully reformed both
methane and biogas although the efficiency was low, on the order of 15% due to excessive slip
and heat losses.
The construction and test of an integrated micro CHP system revealed several problems with the
core technology. Therefore, rather than working with the integrated system, individual system
components were tested separately. In spite of the problems with the reformer and the fuel cell
stack the system was successfully operated and an electric efficiency of 18%LHV was demonstrated.
Page 2
Introduction
The following document presents results achieved through the project Integrated HTPEMFC and
multi-fuel reformer for micro CHP; a development and demonstration project completed under the
ForskEL program through Energinet.dk.
The main report summarizes the main achievements and overall conclusions whereas more
detailed information is given in the supplements.
WP 1: Detailed characterization of HT-PEMFC

The characterization performed under this work package can be summarized under two headings;
single cell tests and stack level tests. Concerning the single cell testing and to some extent also the
stack test, a significant amount of time was spent on the development of characterization
methods.
Application of EIS to cell and stack characterization
At the onset of this project some work existed on the overall characterization of HTPEM single
cells (I,V curves) when operated on hydrogen and to some extent also synthetic reformate gas.
First generation system simulation models existed that would describe this behaviour.
This project has focused on more detailed characterization techniques to improve the
understanding of the mechanisms governing cell performance. The main method that was used is
electrochemical impedance spectroscopy. A detailed description is given in two journal
publications 1 2. The applied test setup consists of an electronic load, either a commercial EIS
system from Gamry interfacing with the load or an in-house LabView code to control the load, and
the single cell with hydrogen and air supplied through mass flow controllers. The setup is
illustrated in Figure 1.
1
J.L. Jespersen, E. Schaltz, S.K. Kr Electrochemical characterization of a polybenzimidazole-based high temperature proton exchange membrane
unit cell. Journal of Power Sources 2009, Vol. 191, Issue 2, 15 June 2009, pp. 289-296, doi:10.1016/j.jpowsour.2009.02.025
2
S.J. Andreasen, J.L. Jespersen, E. Schaltz, S.K. Kr Characterisation and Modelling of a High Temperature PEM Fuel Cell Stack using
Electrochemical Impedance Spectroscopy Fuel Cells 2009, Vol. 9, No. 4, pp. 463-473
Page 3
Figure 1: Single cell test setup applied for Electrochemical Impedance Spectroscopy measurements.
The commercial EIS data acquisition system from Gamry only allowed testing of one cell or stack at
the time and also the ability to develop and test diagnostics algorithms based on the EIS
measurements was limited by the Gamry hardware. Therefore a substantial amount of time was
spent developing a LabView interface to the electronic load that could collect EIS data without the
Gamry system. The concept of the LabView system is shown in Figure 2.
Figure 2: Overall testing procedure applied in the LabView based EIS system.
The resulting data are normally plotted in a so-called Nyquist plot as illustrated schematically in
the left hand side of Figure 3. To assist in the interpretation of the results an equivalent circuit is
often used. It consists of electrical components such as resistors and capacitors to simulate the
electric behaviour resulting from individual cell components as illustrated in the right hand side of
Figure 3.
Page 4
Figure 3: (left) illustration of a Nyquist plot of EIS data and a related equivalent circuit model (right)
relation between cell components / losses and the equivalent circuit.
An example of collected measurements from a real single cell test is shown in the Nyquist plot
shown in Figure 4. As can be seen from the figure, the influence from temperature on the EIS data
is significant showing the ability of the method to capture changes in cell operating conditions.
Figure 4: Nyquist plot of EIS data collected on a single cell at different temperatures.
A large number of equivalent circuit models have been suggested in the literature and a summary
is given in the journal papers. To illustrate the resulting information derived from the models a
plot of the calculated charge transfer resistance as a function of cell operating temperature is
included in Figure 5.
Page 5
Figure 5: Charge transfer resistance as function of temperature derived from equivalent circuit model.
Similar tests were made to map the influence from anode and cathode stoichiometry. As an
example the gas transfer resistance versus air stoichiometry is presented in Figure 6. From this it is
evident that when air stoichiometry exceeds about 3-4 there is limited performance to gain by
further increase of stoichiometry.
Figure 6: Gas transfer resistance as function of cathode stoichiometry.
Measurements were also conducted with simulated reformate gas to investigate the influence
from CO, CO2 and mixtures hereof on cell performance. This work was documented in a
conference paper 3. Similar information can be obtained on stack level as shown in Figure 7.
3
S.J. Andreasen, R. Mosbk, J. R. Vang, S.K. Kr, S.S. Araya EIS characterization of the poisoning effects of CO and CO2 on a PBI based HT-PEM fuel
cell, Proc. Of the ASME 2010 Eighth Int. Fuel Cell Science, Engineering and Technology Conference,FuelCell2010-33054, June 14-16, Brooklyn, New
York, USA
Page 6
Figure 7: Nyquist plot of EIS measurements at four temperatures conducted at stack level.
At stack level the interpretation becomes significantly more complicated requiring more detailed
models. In general the interpretation of the impedance relies on the accuracy of the equivalent
circuit or other type of model. So far relatively simple models were applied. To improve the
physical insight gained from the measurements more mechanistic models must be developed. This
has been the topic of a M.Sc. project 4 in the spring of 2010 and continues through a PhD project
under the COBRA project funded by EUDP.
Development of in-situ sensors
In addition to the capabilities offered by the EIS method an effort was made to develop and test
techniques for in-situ measurements of local cell operating conditions. It was decided to focus on
temperature measurements on both the anode and cathode sides of the MEA. Two concepts were
tested; one with small thermocouples inserted in the bipolar plates through small holes that
almost penetrate the plate and hence touch the MEA surface and another based on thin film
thermocouples deposited directly onto the gasket material. The concept of the former methods is
presented in Figure 8.
4
Jakob Rabjerg Vang, An electrochemical impedance model for HTPEM fuel cells, M.Sc. thesis, Department of Energy Technology, AAU, June 2010
Page 7
Figure 8: Schematic of thermocouples inserted in the bipolar plates on the cathode (left) and anode
(right) sides of the operating fuel cell.
Similar experiments were reported in the literature but in the vast majority of cases, the
thermocouples turned out to severely influence cell operation. The experiments conducted
through this work did show slightly improved cell performance (in contrast to all others where a
poor performance resulted from the thermocouples). The improvement is ascribed to the fact
that a bipolar plate material with better electric conductivity was used in the experiments with
thermocouples imbedded.
To demonstrate the sensitivity of the sensors and the ability to detect changes in operating
conditions tests were made where the cathode and anode supplies were changes (left side of
Figure 9) and the resulting temperature variation recorded (right side of Figure 9).
Figure 9: (left) cathode and anode flow rates versus time (right) resulting temperatures recorded locally
on the MEA.
Page 8
It is evident that both the local variations and the variation with operating conditions were
captured by the sensors. In a long term test there were even some indications that the increasing
losses could be identified from slightly increased heat generation. To confirm this, the possible
influence from heat supplied to the test cell from the heating elements controlling the overall cell
temperature must be eliminated.
Durability studies
A number of tests were conducted on single cell level as well as on complete stacks to study
break-in procedures, steady state degradation and degradation under cyclic operating conditions.
The single cell setup is similar to that shown in Figure 1 only EIS measurements were not
performed.
At the stack level it turned out to be challenging to operate continuously for long periods of time
without interruption. The main source of interruption was unforeseen events in the laboratory
causing power shutdown or interruption of hydrogen supply. Therefore it was decided to move
the stack testing out of the laboratory and into a container located outside the laboratory with
separate hydrogen supply. Figure 10 shows the established test facility that was used for stack
testing.
Figure 10: (left) Interior of container used for long term stack tests (right) Hydrogen supply system with
automatic changeover between hydrogen batteries.
Stack tests were run for just above 6 months with a few interruptions. The longest uninterrupted
periods were each around 2 months. For confidentiality reasons specific test results are not
presented here but detailed information can be found in the confidential supplement. Overall the
degradation levels at single cell and stack levels did not differ significantly. The most important
factor influencing degradation level under steady state operation was the operating temperature.
The experience from the degradation tests combined with information from the literature formed
the basis for a relatively simple simulation model capable of finding the best operating conditions
of the fuel cell given the CO content in the hydrogen feed. Overall the finding was that in long
term operation carbon corrosion was the dominating degradation mechanism. The most
important parameter determining the rate is temperature.
Page 9
When operating on a reformate gas with some amounts of CO, it is desirable to operate at a high
temperature to improve cell performance. Degradation rate and overall performance are thus
counteracting with respect to cell temperature and an optimum operation temperature exists
depending on CO level as illustrated in Figure 11. The details of the work are summarized in a
conference paper 5
Figure 11: End-of-life cell potential after 40.000 hours as function of operating temperature and CO
concentration in the hydrogen feed.
WP 2: Development of multi-fuel reformer

The content of this work package was adjusted as the project progressed as more time had to be
spent on the reactor design due to unforeseen challenges with flow distribution, heat transfer and
flow bypass causing low efficiency and incomplete conversion. Consequently less time was
devoted to the catalyst characterization and modeling as these activities were not as critical as the
core reactor design. The work under WP 2.1 thus mainly focused on the ability to do quantitative
gas analyzes. This activity was shared with a parallel project on methanol reforming (EFP jour.
33033-0211).
WP 2.1 Characterization and modeling of catalyst
A large effort was made to establish the capability to precisely and efficiently characterize steam
reforming catalysts. In this process a number of challenges were faced, the most important being:
5
M.P. Nielsen, S.J. Andreasen, P.L. Rasmussen, S.K. Kr. Experimental study and modeling of degradation phenomena in HTPEM fuel cell stacks
for use in CHP systems. In: Proceedings of the Hydrogen and Fuel Cells Conference (HFC) in Vancouver. Canadian Hydrogen and Fuel Cell
Association, 2009.
Page 10
1. The ability to perform quantitative gas analyses in a reformate stream containing traces of
CO and possibly hydrocarbons in a mixture of H2, CO2 and H2O.
2. The ability to reach sufficiently high and stable temperatures in the test tube reactor.
Many techniques exist to conduct gas analyses and several of these would in theory be capable of
analysing the gas product stream from a steam reforming process. In spite of this, the experience
at the Department of Energy Technology, Aalborg University is that in practical applications a
number of challenges exist. To date three technologies have been applied:
FT-IR with a Gasmet DX4000 (CO, CO2, H2O and H2 from element balance)
Mass spectroscopy with a Pfeiffer OmniStar (detects all gases)
Custom build gas analysis rack from FLS-Airloq (H2, CO, CO2, CxHy)
The FT-IR measurements have been relatively successful but although the analyzer in itself is
insensitive to H2 the readings in reformate streams with high H2 continuous to be problematic
possibly because of internal H2 leakages. In particular the CO measurement caused problems in
these situations but also H2O was problematic obstructing the ability to calculate H2 by difference.
Facing these problems an OmniStar mass spectrometer (MS) was purchased from Pfeiffer Vacuum
as this is capable of detecting all gases in principle down to very low concentrations. The problem
with this device however, is to perform an accurate calibration and to separate gas species with
overlapping spectra with high precision. The factory software is very tedious and time consuming
to use and hence much work has been put into the development of an automatic calibration
system based on LabView. This work was started by Dantherm Power and handed over to AAU for
further development. The current status is such that quantitative measurement can be made
except for CO at low concentrations (less than about 1%vol) but frequent calibration is required.
Figure 12: FT-IR gas analyzer (left) and mass spectrometer (right).
During the process of validating the use of the MS, the Danish Technological Institute brought a
custom made gas analyzer to AAU as a reference for MS measurement that were conducted on a
methanol steam reforming catalyst. From this it was concluded that this system was superior to
the MS and the FT-IR, at least for this specific application. A similar system was configured and
purchased from FLS Airloq by AAU, see Figure 13.
Page 11
Figure 13: FLS-Airloq gas analyzer.
With the three gas analyzers a very good foundation for quantitative characterization of the
reformate gas exists.
The second challenge and major activity concerned the test facility and in particular the ability to
control the reactor temperature and achieve sufficiently high temperatures for steam reforming of
natural gas (required in a parallel ForskEl funded project). At first, attempts were made with a
standard ceramic oven to heat the test section but it proved insufficient in supplying the required
heat. In addition it was not possible to control the heater based on measured temperatures inside
the test section resulting in undesirable temporal variations. Several other attempts were made
before the current setup was designed based on high power radiation heaters. The test section is
equipped with 4 times 750 W heaters that can withstand 1100 C. This has proven very efficient
and enables high and stable test section temperatures. With an in-house LabView control system,
the heaters can be controlled based on thermocouple measurements inside the test section.
Figure 14 shows the test facility with main components to test methanol as well as methane steam
reforming.
Page 12
Figure 14: Photo of the catalyst test facility with main components labelled.
The LabView graphical interface for the test facility is show in Figure 15.
Figure 15: LabView interface for data acquisition and control of the test facility.
Page 13
It was the intention to investigate the deactivation of the catalyst due to impurities such as
sulphur and chlorine and develop modeling tools to predict the behaviour. As mentioned in the
introduction to this work package, the reactor design turned out to be a major challenge and in an
effort to resolve problems related to this the characterization work was abandoned. The activities
related to the reactor design are described under WP 2.2.
WP 2.2 Development of 2nd generation optimized multi-fuel reformer
A component model for the multi-fuel reformer has been developed, to clarify requirements on a
reformer for a 1kWel,net system. Methane conversion and efficiency have initially been fitted to
literature values; intentions were to fit these to experimental data, from reformer tests with
various fuels. A developed reformer thermal model was used iteratively with the initial system
model described in WP3 to ensure boundary conditions used in subcomponent test were suitable.
The thermal reformer model has been revised to clarify thermal and flow changes in the system,
when running on biogas with 40% CO2.
It was decided early that this project should focus on a design, which modulated the reformer
capacity by adding and removing cassettes to and from what is essentially a plate heat exchanger.
Design of the reformer has been based on thermal models and CFD calculations; the amount of
catalyst is by statement from manufacturer oversized by a factor of 4.
A total of four key factors to design an effective and cost effective multi-fuel reformer were
identified and are listed below:
1. High temperature difference on the reactor feed gas
2. Low pressure loss on both fuel feed- and flue gas side
3. High conversion of methane
4. Easy manufacturing
Two different versions were manufactured:

First generation, consisting of 30 cassettes, was laser welded, nicrofer sheet(0,1 mm) and
inconel thin plate(1,1 mm). This version continuously suffered from leaks, as amount of
laser welding was overwhelming to subcontractor
The main conclusion from the first generation reformer was that focus on the ability to
manufacture the reformer was needed, serious leaks made it impossible to conclude on reformer
efficiency/capacity mapping.
Second version consisting of 60 cassettes made of stacking 122 stamped nicrofer sheets
(0,1 mm), with integrated temperature feedback and manifolds, in a brazed construction.
This version was manufactured by Danfoss. Development time was in the range of 1-1,5
years.
With the reformer produced by brazing it was possible to produce a leak-free reformer.
Page 14
During the project it was concluded that to get a successful fuel processing assembly a close
integration between the system burner, the multi-fuel reformer and the integration of the
insulation material was needed.
During reformer development a hybrid conventional and catalytic burner was developed, a total of
10 generations were designed and tested to fit the needs of the multi-fuel reformer heat
requirements and taking expected low content hydrogen fuel into consideration.
A total number of four methods for insulating the high temperature vessels from the surroundings
were tested.
Second and third iterations included attempts on making insulation easier to assemble and mount,
but suffered from too low degrees of insulation.
Fourth version consisted of a return to first iteration, but was only possible after the system had
been changed to fit insulation method.
All in all insulation of the reformer and burner showed to be essential to achieve a high reformer
efficiency and experiences were made that good thermal insulation can be very hard to achieve in
practice.
Flue gas side
After initial test and CFD calculation material from AAU Q4 2009, it was concluded that corrections
were needed on the flue gas side, see Figure 16.
Figure 16: Illustration of region with flue gas bypass.
The corresponding CFD analysis of a single cassette indicating the flow bypass is shown in Figure
17 with the red regions indicating the high velocity bypass flow around the cassette.
Page 15
Figure 17: Illustration of flue gas bypassing the cassettes (red areas corresponding to high gas velocity)
leading to poor heat transfer to the reforming reaction consequently low conversion.
A solution based on indications from CFD calculations was designed and implemented to obstruct
this flow. The effect of these improvements was however masked by introduction of the fourth
iteration of insulation integration, so the effect has only been proven in theory.
Reformate side
Much attention was also directed to the reformate side of the reformer again with particular focus
on flow distribution. The following activities were completed to improve the understanding in this
area:
Detailed experimental characterization of a single cassette with respect to pressure drop

CFD analysis of the entire reformer to predict flow distribution into the cassettes
Flow network modeling to investigate flow distribution and the coupling to reforming
Each of these activities are summarized below and further details can be found in the enclosed
reports.
As reformate gas flow distribution was a key issue experimental characterization of the cassette
pressure loss was conducted as this is critical with respect to the overall distribution between the
cassettes. In addition an investigation of the possible bypass around the wiremesh catalyst was
conducted. To facilitate these measurements a test setup was constructed in the laboratory that
allowed pressure measurements along the reformate gas channel. The setup is illustrated in Figure
18.
Page 16
Figure 18: Test setup used for pressure distribution tests on a single cassette.
The collected pressure distribution data were used to develop pressure loss correlations that were
used in both the flow network model and the CFD model.
The grey area seen in the cassette on the right hand side photo is the wiremesh catalyst. The
catalyst does not fit precisely the width of the cassette. As the thickness of the wiremesh is almost
equal to the channel height a small gap at each side may lead to a bypass flow of reformate
around the wiremesh. To investigate how severe this problem might be a number of investigations
were carried out varying the ratios of wiremesh width to cassette channel width () and wiremesh
thickness to channel height (). Both measurements and CFD analyses were made and the
deviation was within 14%.
Figure 19: Calculated flow distribution around wiremesh at different values of and .
As seen a substantial bypass result from just relatively small gaps at the wiremesh sides due to the
high blockage of the channel height by the wiremesh. More detailed results and discussions can be
found in the enclosed report. Based on this finding it is suggest to avoid too high values of and
the value of must be relatively high corresponding to small gaps at the wiremesh sides.
Page 17
The second analysis that was conducted concerned the distribution between individual cells in the
reformer. Overall the concern was that a too high pressure drop in the manifold distributing the
flow to the individual cassettes compared to the pressure drop in the cassettes would lead to an
uneven distribution and resulting from this a poor conversion. An outline of the CFD model of the
reformer in U-flow configuration is given in Figure 20.
Figure 20: Outline of the CFD model with the flow in U-configuration.
From the calculations it was found that in the best case (U-configuration) with the design manifold
dimension of 10mm diameter the flow through the cassette with the lowest flow was around 25-
30% of that through the cassette with the highest flow. In the worst case around half of the
cassettes have almost no flow (Z-configuration).
This is clearly not acceptable and numerical studies were made to investigate the improvements
achieved by increasing the manifold diameter. With a manifold diameter of 30 mm the U-
configuration has a good flow distribution with a variation between cassettes of only 2-3%. Further
details of the simulations are presented in the enclosed report. The overall conclusion is that the
manifold diameter must be increased to at least 20 mm and if possible even 30 mm.
The CFD based calculations were supported by overall flow distribution modeling with a model
implemented in Engineering Equation Solver (EES). This model is also documented separately in
the supplement. This model confirms the maldistribution between individual cassettes predicted
by the CFD model. The problem is illustrated by Figure 21 showing the relative flow distribution
between cassettes in the reformer.
Page 18
Figure 21: Predicted flow distribution between cassettes in the reformer for U- and Z-configurations.
The simulations were repeated with an increased manifold diameter 3 times the original showed
much improved distributions as seen in Figure 22
Figure 22: Predicted flow distribution with a 3 fold increase in manifold diameter for the U- and Z-
configurations.
There is some disagreement between the CFD simulation results and the prediction from the flow
network model. One predicts more even distribution for the U-configuration whereas for the
other model it is the other way around. The source of this has not been identified in detail but it is
assumed to be caused by complex flow phenomena in the manifold that are not correctly
captured by the flow network model.
The suggested design improvement concerning the manifold was not implemented as it requires
significant changes to the design. Still, it is considered a critical issue with the current design.
FEM analysis
During Q4 2009 FEM analysis on reformer has been performed, it showed that with current
construction and operating parameters the stress in the material does not exceed 62% of the
material design stress. The FEM analysis showed possible improvement with regards to
displacement in the catalyst area.
Page 19
Alternative materials for reformer production (sheet metal) have been identified, purchased and
put on stock; new materials are primary more cost effective and have improved properties with
respect to manufacturability.
Reformer testing
The reformer was tested in a system configuration, close to what is expected of a final system with
methane and biogas as fuel respectively. During the tests on biogas a custom desulphurizer based
on multi-metaloxides were used to address the issue of high sulfur levels in the fuel.
A summary illustration of the tests can be seen on Figure 23 and Figure 24. Key parameters from
the graphs are summarized in Table 1.
It is clearly seen that there is a considerable difference in performance on the two fuels, where the
system performs an order of magnitude better on methane (CH4).
It can also be seen on Figure 24 that at low loads, where the system is able to keep a similar
catalyst temperature, the slip of methane is in the same range. As the load increases, biogas tests
showed that it required more energy and could not maintain a high enough catalyst temperature,
and chemical equilibrium moves towards higher methane slip.
From these results it can be concluded that the system is not able to deliver the 1kWel which was
the design target.
The key problem on the reformer is the methane slip in the reformer, tests on a 60 cassette
reformer concludes that too many parameters are at play and that the conversion rate and
reformer efficiency must be investigated on smaller test samples for example a single cassette, in
order to reach final conclusions.
Key parameters Methane Biogas

Maximum power 365W 253W
Maximum efficiency 17,7%LHV 8,4%LHV
CH4 slip at maximum power 17,1% 29,1%
Table 1 Key parameters from system test on methane and biogas
Page 20
System efficiency and power comparison
20 600
18
16 500
Efficiency[%LHV]
Fuel flow[Nlph]
14 400
12
10 300
8
6 200
4 100
2
0 0
100 150 200 250 300 350 400
P_el_net[W_DC]
CH4 Biogas CH4 fuel flow Biogas fuel flow
Figure 23 System performance of test system, fuelled on methane and biogas
CH4_slip[% input]
40,0
35,0
600
30,0
25,0 550
T_cath[C]
%
20,0
500
15,0
10,0
450
5,0
0,0 400
100 150 200 250 300 350 400
P_el_net[W_DC]
CH4 Biogas T_Cath_CH4 T_cath_biogas
Figure 24 Methane slip and catalyst temperature of test system fuelled on methane and biogas
Page 21
The temperature profile in the reformer varies considerable as well, this is indicated on Figure 25 it
is seen that a smaller temperature difference and thereby a lower catalyst temperature is
obtained in the case where biogas is used as fuel.
Reformer temperature profile 250 el net yield
700
650
600
Temperature[C]
550
500
Catalyst area
450
400
350
0 2 4 6 8 10
Position(not physical)
Reformer profile CH4 1(250W) Reformer profile CH4 2 (250W)

Reformer profile biogas (250W) Reformer profile biogas (250W)
Figure 25 Temperature profile in the reformer
Conclusions on WP2.2
Energy modeling and CFD calculations were used to design and evaluate two versions of a
reformer. Although it was not possible to correlate test results with models, the models aided
engineers in the design phase and gave insight when analyzing obtained results.
A large number of model simulations of varying complexity were conducted to analyze different
sub problems mainly related to flow distribution issues. Bypass around the sides of the wiremesh
catalyst was found to be a potential problem. A second area of major concern is the manifold
diameter that is too small leading to uneven distribution between individual cassettes in the
reformer.
From these investigations it was also concluded that thermal modeling and CFD calculation must
be correlated at a physically much smaller scale for example a single cassette, especially because
in this project, the achieved and expected outcome differ quite a lot.
Although several improvements were suggested to the design, the multi-fuel reformer successfully
reformed methane and biogas.
Page 22
AP 3: Development of integrated micro CHP system
The goal of this work package is to implement the comprehensive optimization of system design
and system integration so as to achieve a robust, inexpensive and ultra compact system. This will
be done based on existing experience and especially on results of the developed simulation models.
The scope of this work package quickly adjusted due to the performance issues on the reformer.
System optimization is not relevant, when core technology is not performing up to specification.
Therefore the work conducted under WP3 at Dantherm has ended up being concentrated on initial
system modeling and later on, in the more implementation oriented part of the work package, to
getting a suitable test platform for the multi-fuel reformer and closely related components, rather
than optimizing the system as a whole.
Aalborg University has developed a system simulation model that can be used to analyze different
operational strategies of the system and the resulting efficiency. It was decided to base the model
on Labview since it would allow coupling with experimental testing and it is available in the
Dantherm Power. The model is described in detail in a separate enclosed report.
Development
Models to clarify system requirements, when integrating a reformer for a 1kWel,net system have
been developed. System models helped predict performance targets and the component level
approach, facilitated an easy way of ensuring boundary conditions on subcomponent test were in
the correct range.
System models have been revised to clarify thermal and flow changes in the system, when running
on biogas with 40% CO2. This indicated that the heat transfer required in the reformer would have
to be 6,4% higher when operating on biogas and that the extra flow of CO2 would result in an
increase in pressure drop of 25%. Likewise it was concluded that the heat transfer required in the
gas clean-up stage would have to be 26% higher compared to operation on pure methane.
Initial system design focused on utilizing the expected high tolerance of the HTPEM fuel cells to
keep reformate clean-up and system design as simple as possible. During test at Dantherm and
Serenergy it was however concluded that this simple system design was not suitable for use with
the HTPEM fuel cells, especially the non-operational conditions feasible in such a design showed to
be insufficient. Close cooperation with stack module manufacturer was established to come to a
suitable operational procedure.
Development of the system to facilitate test on the multi-fuel reformer have concentrated on
getting a suitable test platform, ensuring reliable and sufficient data from test. This mainly
consisted of automating controls of system to get few inputs for test operator.
Page 23
Tests
Tests on reformer were performed in the developed system, the system components have been
initially evaluated for performance. A possible optimization point seems to be the characteristics
of the air supply to burner supplying high-enthalpy energy to the reformer.
For final tests on methane and biogas an auxiliary air supply for the burner was used to get a good
mapping of the core technology.
During the final tests several manual operations were performed to live up to stack module
manufacturers operational procedure, again verifying the need for a more advanced system
integration with lower demands to stack module robustness.
Conclusions from AP 3
Development of a test system for the core technology was conducted. The test system enabled the
core technology to be tested in a system quite close to the configuration of a suitable CHP
system of 1kWel. The system as a whole did not meet the listed expectations on electrical
performance; the thermal performance was not investigated as electrical performance is the
driving force of fuel cell based CHP systems. Maximum achieved electrical power was 360WDCnet
with an efficiency of 17,7%LHV
Communication of project results

The results of this project were presented in a number of scientific papers that are enclosed with
this report:
J.L. Jespersen, E. Schaltz, S.K. Kr Electrochemical characterization of a polybenzimidazole-based

high temperature proton exchange membrane unit cell. Journal of Power Sources 2009, Vol. 191,
Issue 2, 15 June 2009, pp. 289-296, doi:10.1016/j.jpowsour.2009.02.025
S.J. Andreasen, J.L. Jespersen, E. Schaltz, S.K. Kr Characterisation and Modelling of a High
Temperature PEM Fuel Cell Stack using Electrochemical Impedance Spectroscopy Fuel Cells 2009,
Vol. 9, No. 4, pp. 463-473
S.J. Andreasen, R. Mosbk, J. R. Vang, S.K. Kr, S.S. Araya EIS characterization of the poisoning
effects of CO and CO2 on a PBI based HT-PEM fuel cell, Proc. Of the ASME 2010 Eighth Int. Fuel
Cell Science, Engineering and Technology Conference,FuelCell2010-33054, June 14-16, Brooklyn,
New York, USA
M.P. Nielsen, S.J. Andreasen, P.L. Rasmussen, S.K. Kr. Experimental study and modeling of
degradation phenomena in HTPEM fuel cell stacks for use in CHP systems. In: Proceedings of the
Hydrogen and Fuel Cells Conference (HFC) in Vancouver. Canadian Hydrogen and Fuel Cell
Association, 2009.
Page 24
List of enclosed material
Enclosure A: SerEnergy Test Report A summary of completed testing, Serenergy A/S 2008
Enclosure B: Investigation of flow properties in single reformer cassette using experiments and
numerical simulation, Haftor rn Sigurdsson, Department of Energy Technology, AAU, 2010
Enclosure C: Flow distribution through the 60 plate steam reformer manifold, Department of
Energy Technology, AAU, 2010
Enclosure D: Fundamental modeling of the plate heat exchanger multifuel reformer to assess
maldistribution, Mads Pagh Nielsen, Department of Energy Technology, AAU, 2010
Enclosure E: Modeling and operation of a HT-PEMFC based micro-CHP system in LabVIEW,

Alexandros Arsalis, Department of Energy Technology, AAU, 2010
Page 25

Integrated HT-PEMFC and Multi-Fuel Reformer For Micro CHP

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Integrated HT-PEMFC and multi-fuel reformer

for micro CHP

Program theme: Fuel Cells

Project summary .............................................................................................................................. 2

WP 1: Detailed characterization of HT-PEMFC ................................................................................ 3

Application of EIS to cell and stack characterization ................................................................... 3

Development of in-situ sensors ................................................................................................... 7

Durability studies ......................................................................................................................... 9

WP 2: Development of multi-fuel reformer................................................................................... 10

WP 2.1 Characterization and modeling of catalyst .................................................................... 10

WP 2.2 Development of 2nd generation optimized multi-fuel reformer ................................... 14

Flue gas side ............................................................................................................................... 15

Reformate side ........................................................................................................................... 16

FEM analysis ............................................................................................................................... 19

Reformer testing ........................................................................................................................ 20

Conclusions on WP2.2 ................................................................................................................ 22

AP 3: Development of integrated micro CHP system .................................................................... 23

Conclusions from AP 3 ............................................................................................................... 24

Communication of project results.................................................................................................. 24

List of enclosed material ................................................................................................................ 25

Published Papers ................................................................................................................................

Figure 6: Gas transfer resistance as function of cathode stoichiometry. ............................................ 6

Figure 13: FLS-Airloq gas analyzer...................................................................................................... 12

Figure 16: Illustration of region with flue gas bypass. ....................................................................... 15

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Figure 25 Temperature profile in the reformer ................................................................................. 22

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

A number of experimental characterization methods were developed through this project to

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

WP 1: Detailed characterization of HT-PEMFC

Application of EIS to cell and stack characterization

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Figure 6: Gas transfer resistance as function of cathode stoichiometry.

Development of in-situ sensors

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

WP 2: Development of multi-fuel reformer

WP 2.1 Characterization and modeling of catalyst

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Figure 13: FLS-Airloq gas analyzer.

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

WP 2.2 Development of 2nd generation optimized multi-fuel reformer

Two different versions were manufactured:

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Flue gas side

Figure 16: Illustration of region with flue gas bypass.

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Detailed experimental characterization of a single cassette with respect to pressure drop

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

Key parameters Methane Biogas

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark

System efficiency and power comparison

CH4 Biogas CH4 fuel flow Biogas fuel flow

Figure 23 System performance of test system, fuelled on methane and biogas

CH4 Biogas T_Cath_CH4 T_cath_biogas

Institute of Energy Technology Pontoppidanstrde 101 9220 Aalborg Denmark