EFFECT OF CONTAMINATION TOWARDS PROTON

EXCHANGE MEMBRANE FUEL CELL

PERFORMANCE: A REVIEW ON MODELING AND
SIMULATION WORKS

Muhammad bin Lebai Rodin

Saiful Hasmady bin Abu Hassan, Dr.
Contents
Abstract ................................................................................................................................................... 3
1.0 Introduction ....................................................................................................................................... 3
2.0 Review on PEMFC Contamination................................................................................................... 5
2.1 PEMFC modelling and simulations without contamination ......................................................... 6
2.2 PEMFC modelling and simulations with contamination .............................................................. 9
2.3 Summary ..................................................................................................................................... 10
3.0 Conclusion ...................................................................................................................................... 10
4.0 References ....................................................................................... Error! Bookmark not defined.

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Abstract
Proton exchange membrane fuel cell (PEMFC) is a well-known energy converter that has the advantage
of low greenhouse gases (GHG) emission, low operating temperatures, and high power density. PEMFC
operates on hydrogen (H2) as fuel, and oxygen (O2) as oxidant. Inverse electrolysis occurs between the
oxidant and the fuel. As a result, water (H2O) forms as their by product. In practical, O2 is supplied from
the free air. However, the free air contains not only oxygen but also other gases such as sulphur dioxide
(SO2), and nitrogen oxides (NOx). On the other side, the H2 fuel may contain traces of carbon monoxide
(CO) as a result from its previous reforming process. This makes PEMFC susceptible to disruption from
these foreign particles. These contaminating gases from the free air occupy the reacting sites originally
meant for O2 and react with hydrogen ions instead of oxygen ions. Meanwhile, small portion of CO
traces from the fuel occupies the reacting sites for H2 and react with oxygen ions instead of hydrogen
ions. Consecutively, the energy output from the PEMFC will be short from its expected numerical value
resulting in a less efficient PEMFC. Hence, this paper reviews recent research on PEMFC under the
impact of cathode and anode side contaminants, in particular via modelling and simulation. This
comparative review serves to find out potentials in improving PEMFC operation, broaden its
practicality, and solving its mitigation strategies.

1.0 Introduction
Growing population has been observed in previous decades. This occurrence incites increasing demands
in energy consumption as communities rely on energy to run most of their daily activities. Common
energy consumptions include transportation, electricity, heat houses, and industrialization. Hence, the
energy industry has been urged to produce and supply more energy to keep up with the growing demand.
Currently, the main energy production source is from fossil fuels. Fossil fuels are very old and require
hundreds of million years to deposit and be rendered useful. With the wide-scale extraction of fossil
fuels, they are considered as finite source. Vast consumption of fossil fuels has led the globe into an
accelerating depletion of the finite source of energy. Concurrently, growing population increases fossil
fuels depletion rate.
On the other hand, fossil fuels also threatens the environment with its harmful and not
disposable by products. Fossil fuels produce by products such as CO2, CO, and SO2. These gases
represent GHG. In the long term, these gases lead to worldwide problems such as, global warming,
rising sea level, and climate change. Hence, initiatives have been taken to find alternatives to secure
and sustain energy supply which promises cleaner methods. Examples of such cleaner approaches
include renewable and hydrogen energy.
Hydrogen is capable of being utilized freely as it is a chemical energy carrier. However, current
sources of hydrogen is mainly from fossil fuels. Hence, different methods of hydrogen production are
deemed to be utilized. Current decent methods are reforming and electrolysis. Comparing the two,
electrolysis tops reforming in terms of cleaner method as reforming produces harmful by products.
Electrolysis is also considered as a renewable method to produce hydrogen.
Some possible methods of hydrogen production are distinguished from renewable and non-
renewable. Multiple recent research have been done on these conventional or non-renewable and
renewable methods by comparing environmental impacts, production cost, and energy and exergy
efficiencies [1]–[3]. Thermochemical splitting with the Cu-Cl and S-I cycles is good for environment
in terms of emission as shown in Figure 1. Wind, solar, and high temperature electrolysis are also good
for environment but has high cost as shown in Figure 2. Biomass gasification has good energy and
exergy efficiency as shown in Figure 3. It was also proved that thermochemical pyrolysis and
gasification are economically viable. Biological methods are promising but need more research studies
to improve production rate. Low conversion efficiencies and high investment costs restricts water-

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splitting technologies. However, when using fossil hydrocarbons, precautions must be taken to extract
and sequestrate CO2.

Figure 1 - SCC of selected hydrogen production methods (per kg of hydrogen) [1].

Figure 2 - Average production cost of selected hydrogen production methods (per kg of hydrogen) [1].

On the other hand, new technologies on electrolysis have been discussed in terms of power
system [4], design [5], and resistance analyses [6] in recent studies. Recent studies on hydrogen
production by reforming have also been done by several scholars [7]–[10] even though it poses threats
as much as fossil fuels do.
Other innovation in hydrogen production was studied by introducing a new concept called 18S;
source, system, service, scope, staff, scale-up, safety, scheme, sector, solution, stakeholder,
standardization, subsidy, stimulation, structure, strategy, support, and sustainability. The innovative
methods were compared and evaluated by using a ranking method. Geothermal and biomass has the
highest sustainability followed by hydro and solar. Coal has the lowest sustainability followed by
nuclear and natural gas. Thermochemical is on top of the ranks in terms of hydrogen production system
followed by photofermentation and artificial photosynthesis. Photoelectrochemical is lowest followed
by photocatalysis and thermolysis [11].

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 Figure 3 - Energy and exergy efficiencies of selected hydrogen production methods [1].

Figure 4 - Schematic of the designed electrolytic cell: (a) electrolytic cell and electrolysis; (b) side view of the electrolytic
cell; (c) upper view of the electrolytic cell; and (d) separation plate between electrodes [5].

2.0 Review on PEMFC Contamination

Fuelling on hydrogen alone, a PEMFC has high power density, and it operates at low temperature. A
PEMFC consists of seven layers which are membrane, catalyst layers (CL), gas diffusion layers (GDL),
and gas channels (GC). CLs sandwiches the membrane in the middle followed by GDLs and GCs. The
fuel which is H2 enters on the anode side while the oxidant which is O2 enters on the cathode side. O2

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discharges into oxygen ions and reacts with hydrogen ions crossing the membrane layer and forms
water (H2O) and exits on the cathode side.
However, it is susceptible to contamination from CO on the anode side and NOx and SO2 on
the cathode side. The questions are, how the contaminants affect the kinetics of both the anode and
cathode side of the fuel cell and how to correlate the PEMFC performance with the contamination.
Recent developments in PEMFC has been studied. Wu et al. [12] reviewed past technical papers
on transport and performance modelling of PEMFC to highlight valid findings on the topic for the
benefit of improving transport and performance of PEMFC in the coming years. The review was done
of papers only from 2010 to 2015 to ensure that the findings were acceptable and not yet expired of the
fuel cell growth. The study focused on the characteristics of transport in membrane, catalyst layer, gas
diffusion layer, and channel.

2.1 PEMFC modelling and simulations without contamination

With assistance from CFD, modelling and simulation of a PEMFC has never been easier thus
forwarding to several studies in this matter. Kone et al. [13] presented a comprehensive CFD tool to
simulate transport processes in PEMFC to improve its performance and efficiency. They utilized
OpenFOAM to develop a model of PEMFC and study further on the inside processes of the fuel cell
and compared the results with previous model and experimental results. Current results showed a better
agreement I-V curve with experimental curve at low current densities. Concentration constant has
significant effect on the concentration overpotential. Figure 5 shows the geometry and mesh of a single
PEMFC that has been designed.

Figure 5 - Geometry and mesh of a single PEMFC [13].

Haghayegh et al. [14] modelled and examined an isothermal, 3D, single phase PEMFC with
serpentine flow using a FEA in COMSOL Multiphysics 4.0 with equation based modelling, meshing
abilities, and various solvers. They solved mass, momentum, and electrochemical equations
simultaneously for steady state condition and compared the numerical results with experimental results
collected from fabricated MEA. Numerical results are acceptable when compared with experimental
results. Higher current density was predicted for the catalyst with a bigger surface area and Pt content.
Oxygen, hydrogen, and water mass fraction distribution, velocity magnitude, and pressure distribution
was estimated and effects of temperature and pressure on current density was predicted.
Falcao et al. [15] compared 1D and 3D simulations to identify the advantages and disadvantages
of both types and studied the effects of 2 phase flow, reactants humidity, and operating temperatures
using ANSYS FLUENT. The results were shown by polarization curve in Figure 6, membrane water
content, and protonic conductivity in Figure 7. Comparing the simulations of 1 phase of 1D and 3D and
2 phase of 3D model with experimental data, 1D model topped the 3D model by shorter rendering time

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while the results were similar. 3D simulation with 2 phase flow showed better results visualizing the
water liquid formation blocking the pores thus reducing the performance of the fuel cell. Results showed
that the relative humidity supports the performance of the fuel cell. Performance of the fuel cell slightly
increase with the operating temperature. Protonic conductivity increases as the operating temperature
increases.

Figure 6 - Comparison between experimental data and 3D numerical simulations of polarization curves for the three
temperatures studied: (a) 298K; (b) 313K; and (c) 333K, both gases relative humidity of 95% [15].

Figure 7 - Protonic conductivity along the membrane predicted by the 1D model for 0.6V and for the three studied
temperatures: (a) 298K; (b) 313K; and (c) 333K, both gases relative humidity 95% [15].

Valencia et al. [16] used ANSYS 15.0 in modelling a single-phase, 3D PEMFC to simulate the
fluid flow, heat transfer, electrochemical reaction, and species transport. Results showed that the species
concentration was always higher at the inlet then descended as it gradually conveyed along the channels
whilst temperature was lowest at the inlet. The results were verified from the polarization curve and
experimental data from previous research. It was concluded that the model can be used in the nearest
future to improve the stack design and cooling method.
Qin et al. [17] modelled a 2 phase flow for the cathode side in a PEFC using ANSYS FLUENT.
The GC was set to be a structured porous medium with a porosity of 1.0. 2 phase Darcy’s law was
applied to the DL and the GC. The effect from immobile saturation on the liquid water distribution in
the DL was studied. Results showed that the ignorance of water flooding the GC will affect the

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prediction of liquid water distribution in the DL and overestimation of the cell performance. It was also
found that decreasing the relative humidity of the inlet gas can reduce the flooding of the GC
considerably to also avoid the membrane from being dehydrated.
Chavan et al. [18] modelled a simple but realistic PEMFC in MATLAB SIMULINK to evaluate
its performance with different operating conditions such as hydrogen flow rate, hydrogen humidity, and
hydrogen partial pressure. The results of the model was compared to an experimental data from a single
25 cm2 PEMFC which can be also collected from a stack of several cells. The results from the model
and the experimental prototype visualized by polarization curves showed a good agreement with nearly
matching pattern.
Salva et al. [19] optimized the operating conditions of a 50 cm2 PEMFC by modelling in 1D
with validation from experimental data according to the cell temperature, pressure, reactants relative
humidity, and cathode stoichiometry. The model was used to predict the operating conditions that result
in maximum and minimum power output for different current intensities. Results on the operating
conditions to maximum and minimum power output were obtained and showed good agreement with
the experimental data with errors of 2% and 3% respectively. The comparison showed that the
maximum is about 100% higher than that of the minimum.
Abidin et al. [20] modelled an advanced 1D PEMFC in Matlab-Simulink based on physical
parameters to predict the overall behaviour of the fuel cell with planned energy system which can also
be utilized to simulate an existing energy system for research purposes. The research was also carried
out to use the model to predict the effects of varying design parameters, materials, and environmental
conditions cutting the cost in terms of time and expenses. It was found that temperature affects the
cell’s performance more than pressure does shown in the polarization curves from the model. It was
also found that a sufficient humidification level is essential. If the membrane is not properly hydrated,
the anode-membrane interface will eventually have an increasing ionic resistance, or worse,
permanent damage.
Sierra et al. [21] designed a 3D PEMFC with 3 different cylindrical geometry flow fields;
serpentine, interdigitated, and straight channels to study the performance of the fuel cell with each flow
field geometry. Conventional flow field geometries inflict pressure losses with rectangular geometry.
Modelling was done with commercial CFD code. Pressure losses, species concentration, current
density, temperature and ionic conductivity were studied from the fluid mechanics equations and
electrochemical model of Butler-Volmer. Results were obtained at the GC, CL, GDL, and membrane
showing that cylindrical channel geometry decreased the pressure losses. Results from the model was
also compared to literature data and polarization curves of similar designs thus proving that this design
tops the conventional rectangular designs in terms of uniform pressure, and current density
distributions.
Saeed et al. [22] analysed a renewable PEMFC system by classing the PEMFC into 4
subsystems; fuel cells as the power source, electrolyzer to produce hydrogen, photovoltaic modules as
the renewable source to provide the electrolyzer, and hydrogen tank. Then, each subsystems were
modelled in MATLAB to obtain the operational curves which then were used to design a 1kW fuel cell
system by calculating the amount of hydrogen needed to run the fuel cell, size of the electrolyzer to
produce the corresponding amount of hydrogen, the energy required by the electrolyzer, estimating the
power from the PV modules to provide the energy required with respect to Damascus’ solar irradiance,
and the size of the hydrogen tank to assist the fuel cells for the whole year, tentatively. Even though the
system is independent and sustainable, it is still complex, expensive, and not on par with the current
available power plant. As an alternative, the system could be used as a backup system storing excessive
energy in the form of compressed hydrogen.

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 Figure 8 - The contribution of overpotentials to the polarization curve [23].

However assisting CFD can be in modelling and simulating, there will always be rooms for
improvement in the technology of such dynamics. Bednarek et al. [23] studied limitations and
challenges in PEMFC modelling in CFD and strategies to counter them. They simulated polarization
curve at steady-state conditions and the effects of fuel cell components on the overpotentials were
shown on the polarization curve in Figure 8. Investigation on potential losses due to ohmic and mass
transport limitations, and the effect of the exchange current density and open current voltage were also
done. Insufficient and robust input data were identified as the reason to inaccurate results shown with
respect to: (1) velocity, temperature, and pressure distribution; (2) concentration of reactant species; (3)
accumulation of water vapour in the GDL and membrane. They compared water vapour balance and
species distribution from CFD and analytical calculations which then ended up in an acceptable manner
from both methods. The study also concluded that the liquid water in the GC does not influence the
flow rate of the species.

2.2 PEMFC modelling and simulations with contamination

Sethuraman et al. [24] studied the effects of sulphur poisoning on Pt catalysts in hydrogen oxidation
reaction (HOR) using functional PEMFC. From the experiment, H2S supplied at 70 oC deactivated 6%
of Pt reaction area even after removal. The deactivation was worse when the test was done while the
fuel cell was running with finite load. Polarization curves did not show any losses in performance of
the fuel cell suggesting that the curves cannot be used to assess the recovery rate of the sulphur
poisoning. A mechanism was presented to visualize the reaction of adsorption and electro-oxidation of
H2S on Pt anode. H2S adsorbs onto Pt in two different species which then electro-oxidizes into sulphur
and then to sulphur dioxide. The ignition of oxidation of sulphur dioxide decreases with higher
temperature. Combining with faster electro-oxidation kinetics eases the removal of adsorbed sulphur.
It was concluded that the exposure of PEMFC to H2S should be kept below equilibrium potential of
sulphur oxidation to avoid any possibility of permanent loss of Pt sites.
Zhai et al. [25] investigated the effects of different temperatures on SO2 contamination in a
PEMFC operating at 2ppm SO2 in the cathode. It was done to understand the mechanism of SO2 in
contaminating the fuel cell. As the contaminant accesses the fuel cell through the diffusion in GDL and
CL in the cathode, water management holds an important task in varying the water level in the fuel cell.

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The experiment was done by exposing the fuel cell with 2ppm of SO2 which then followed by neat air
recovery and CV scanning. The fuel cell was then again exposed to the same 2ppm of SO2 to determine
the efficiency of the recovery processes and also to study the re-poisoning processes. As it turned out,
recovery process at low temperature was low by neat air. However, CV scanning obtained full recovery.
It was also found that increasing the water level in MEA delayed the poisoning effect at low
temperature. Sulphur adsorbates were failed to be decomposed/desorbed at low temperature. At low
temperature, SO2 crossover from cathode to anode was reduced.
Ge et al. [26] studied effects of acetylene, C2H2 on oxygen reduction reaction (ORR) for a Pt/C
catalyst using rotating ring disc electrode (RRDE) in acidic solution. The objective of the study was to
look into how acetylene contaminates the cathodes in PEMFC. Cyclic voltammetry results showed an
almost complete loss of electrochemical surface area covered by acetylene with concentration of
0.14mM. Using RRDE to measure the polarization curve, a presence of acetylene shifted the potential
in the negative direction by 330mV which can be identified as a result from the loss of electrochemical
surface area on Pt/C catalyst.
Reshetenko et al. [27] studied experimentally and analytically on the spatial performance of
PEMFC and also its spatial electrochemical impedance spectroscopy (EIS) responses from the presence
of low concentration CO. Using air, O2, and H2 to fuel the fuel cell, several results were obtained. CO
adsorption on the anode and its poisoning reduced the voltage. Running the cell with air/H2 and H2/H2
configuration, a pseudo-inductance behaviour was noticed in the low frequency region for inlet
segments. Using O2 as oxidant did not induce a pseudo-inductance behaviour. The EIS and anode
overpotential data was analysed and it was proposed that the CO oxidation occurs chemically or
electrochemically or a combination of both with respect to the operating gases.
Chen et al. [28] studied the poisoning of NOx on oxygen reduction reaction (ORR) at Pt/C
catalyst for PEMFC by 3-electrode method in liquid electrolyte solution. Cyclic voltammetry (CV)
results verified that the NOx is more significant with metallic Pt compared to Pt oxide and that the
reaction is chemical rather than electrochemical. Linear sweeping voltammetry (LSV) results showed
that the absorption of NOx degrades the performance of Pt/C catalysts due to the decreasing reaction
area available for oxygen to be exposed to. It was found that by reducing the working potential is
capable of mitigating the NOx poisoning due to the fact that NOx is reduced by lower potential.

2.3 Summary
Windows for improvements in technological growth nowadays are always open and available. Hence,
from the reviews above, it is advisable that more research on fuel cells should be accomplished. In the
literature, there are minimal detailed findings on contamination in certain particular gases. Answering
the objective of this paper, it is viable to study on how sulphur dioxide reacts with the catalyst layer on
the cathode side.
On the other hand, it would also be beneficial for future studies to prepare a multicomponent,
which in this case a quaternary gas module, as it is also an angle which very few to none research have
been done. Further to the research, the module will be modelled by using OpenFOAM open source
software. Controlling the operating parameters, a parametric study is amenable.
Finally, discussions and suggestions on the mitigation strategies will be done to improve the
performance of the PEMFC and help comprehend the contamination of SO2.

3.0 Conclusion
For the conclusion, it is viable to do such research to fill in the gap in the corresponding field of study.
Studies on the contamination of SO2 in the cathode side of the PEMFC is minimal as well as the
approach to prepare a multicomponent gas module for future experiments involving multiple species of
gases.

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