international journal of hydrogen energy xxx (xxxx) xxx

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Review Article

Review of gas diffusion layer for proton exchange

membrane-based technologies with a focus on
unitised regenerative fuel cells

Reza Omrani, Bahman Shabani*

School of Engineering, RMIT University, Australia

article info abstract

Article history: Proton exchange membrane (PEM) based technologies (fuel cells and electrolysers) offer
Received 15 October 2018 promising sustainable power generation and storage solutions for a diverse range of sta-
Received in revised form tionary and mobile applications. Unitised regenerative fuel cell (URFC) is an electro-
10 December 2018 chemical cell that can operate both as a fuel cell (FC) and an electrolyser (E). However, for a
Accepted 17 December 2018 widespread commercialisation, further improvements are required that address the
Available online xxx durability, performance, and cost limitations. One of the main challenging components in
developing URFCs is the gas diffusion layer (GDL) as it plays different vital roles, some of
Keywords: which are paradoxical in FC and E-modes. Therefore, in this paper, the published research
Gas diffusion layer on GDL of PEM-URFCs as well as relevant studies on PEM fuel cells and electrolysers are
Unitised regenerative fuel cell critically reviewed. The materials and novel methods to address the corrosion in E-mode
Electrolyser are discussed. This is followed by presenting and discussing different properties of GDLs
PEM affecting the performance in FC and E-modes: i.e. porosity, thickness, pore size, transport
GDL properties, thermal and electrical conductivity, and the GDL compressibility. Finally, the
main modifications of the GDLs, such as hydrophobisation and microporous layer appli-
cation, to improve the performance of a URFC are analysed and discussed.
© 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Contents

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
GDL materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Hydrogen side GDL material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Oxygen side GDL material . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Carbon paper and carbon cloth comparison . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
GDL properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Overview . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Porosity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Thickness . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00

* Corresponding author.
E-mail addresses: reza.omrani@rmit.edu.au (R. Omrani), bahman.shabani@rmit.edu.au (B. Shabani).
https://doi.org/10.1016/j.ijhydene.2018.12.120
0360-3199/© 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
2 international journal of hydrogen energy xxx (xxxx) xxx

Pore size distribution . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00

Transport properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Diffusivity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Permeability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Thermal properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Electrical properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
GDL compressibility and stack assembly . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Modifications of GDLs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Overview . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Hydrophobisation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Micro porous layer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 00

URFCs are lighter and smaller than a separate electrolyser and

Introduction
The global energy demand is predicted to experience a 37%
growth by 2040 compared to its level in 2014 [1] making it one
of the highest priority concerns at a global level. This increase,
if not addressed effectively through energy efficiency and
sustainable practices, can have significant environmental
impacts while leaving a considerable stress on the infra-
structure [2,3]. Therefore, renewable energy sources must
have an increasing role in the global energy supply [4,5]. In
sustainable energy strategies, hydrogen can play a crucial role
[6e8] as it can be utilised in a wide range of applications such
as for vehicles [9e11], satellites [12], telecommunication sta-
tions [13e15], and remote area power supply [16e20] to name
a few. In addition, hydrogen can be used to overcome the
intermittent nature of renewable energy resources and facil-
itate their integration into the network [21,22]. Dissimilar to
batteries, hydrogen storage does not suffer from self-
discharging making it is desirable for long-term (e.g. sea-
sonal) energy storage applications [17,23e26] or applications
in extreme hot or cold climatic conditions [27].
Polymer electrolyte membrane (PEM) fuel cells (FCs) are
electrochemical devices converting the stored energy in
hydrogen into electricity. PEMFCs provide several benefits
such as high efficiency and energy density, simplicity, and
quick start-up [28]. However, PEMFCs are dependent on con-
stant external hydrogen supply [29], i.e. they are open-loop
systems. Therefore, application of PEMFCs needs an infra-
structure for H2 production and distribution facilities that may
not be economical for all instances. One solution to this issue
is regenerative fuel cell (RFC) system (Fig. 1a), which is a
combination of a PEMFC and a PEM electrolyser, forming a
closed-loop rechargeable system [30]. Therefore, an RFC sys-
tem stores electrical energy in form of hydrogen, which will be
used when needed by the PEMFC (see Fig. 2).
In practice, currently, RFC systems are mainly used for
military and space applications due to their high cost and
complexity [31,32]. Unitised regenerative fuel cell (URFC) sys-
tems have been developed (Fig. 1b) to address the space and
mass limitations, where these are the main constraints. Hence
fuel cell (RFC) system [29,33]. URFC systems can be used in
microgrid networks for storage and feed of energy in order to
reduce the operational cost [34]. Other possible applications
proposed for URFCs are for: standalone hybrid power supply
[35e37], load levelling [38], and transportation [39e41].
The main components of a PEM-URFC stack are bipolar
plates (BPP), gas diffusion layer (GDL), catalyst layer (CL),
membrane, and gasket as presented in Fig. 2. Bipolar plates
accommodate the flow field channels to take the reactants to
the cell and remove the products while conducting the elec-
trons and heat. In PEM electrolysers and URFCs, BPPs are
mostly made of titanium (Ti) coated by platinum (Pt) or gold
(Au) to provide long-term durability and improved corrosion
resistance as well as lower electrical resistance [42e47].
However, development of URFCs faces some challenges
that have to be addressed in order to take them to the com-
mercialisation stage [49e51]. One of the most important of
these challenges is the corrosion of the GDL in electrolyser-
mode (E-mode), which acts as a distributor between flow
channels and active area (catalyst layer). The main roles of
GDL in a PEM-URFC are providing [52,53]:

a pathway for the reactants, i.e. oxygen and hydrogen in
FC-mode and water in E-mode, to move from the flow field
channels toward the CL and be distributed evenly over
there, especially under the ribs;

an effective capacity for the removal of the products (water
in FC-mode and oxygen and hydrogen in E-mode) from the
CL to the channels;

a structural support to the MEA under the assembly pres-
sure and differential pressure between oxygen and
hydrogen sides in E-mode and preventing it from intrusion
into the channels;

an electrical connection between the BPPs and the CL; and

a thermal pathway to transfer the heat generated at the CL
to the BPP, where the heat will be removed from the cell.
Therefore, the GDL should have the following optimal
properties that are specific to the cell design: gas and vapour
diffusivity and permeability, porosity, surface contact angle,

Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
 international journal of hydrogen energy xxx (xxxx) xxx 3

Fig. 1 e Comparison of (a) discrete and (b) unitised regenerative fuel cell systems [30].

Fig. 2 e Schematic exploded view of (a) single-cell PEM-URFC; (b) MEA; (c) dual-layer GDL [48].

Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
4 international journal of hydrogen energy xxx (xxxx) xxx
electrical and thermal conductivity, mechanical strength, and
durability in PEM electrolyser environment at the required
operating conditions [52,54].
The conventional GDLs that are usually carbon-based and
used in PEMFC applications suffer from rapid and severe
corrosion at the oxygen side in electrolysis environment; this
makes them unsuitable for use in PEM URFCs [55,56]. There-
fore, in URFCs, mostly porous titanium products are used
[57e61] or protective layers are applied to conventional
carbon-based GDLs with limited success [55,56,62]. Several
studies have shown the effect of different properties of the
GDL on the overall performance of PEMFCs [58,60,63e86].
However, these studies are mostly focused on carbon-based
GDLs (CGDLs) while the role of GDL in URFCs has been
addressed in a few papers to a limited extent [58e60].
Having more insight into the role of GDL in PEMFCs in
general and URFCs in particular (the latter has not been
investigated much in the literature), can help identify possible
pathways for further research and development on the design
of GDLs to enhance both performance and durability. There-
fore, the present paper provides a comprehensive review of
the above-mentioned topic that can contribute to the research
and development of URFC technologies. In this paper, it has
been tried to present the findings from the research studies
carried out to date on the GDLs used in URFCs as well as
PEMFCs and PEM electrolysers separately that are also appli-
cable to URFCs.
Initially, suitable materials for GDLs used in URFC are dis-
cussed both for hydrogen and oxygen sides. For the oxygen
side, various methods used by different researchers to inhibit
the carbon corrosion are also reviewed. This is followed by
presenting and discussing different GDL properties affecting
the URFC performance in FC and E-modes, including porosity,
pore size distribution, thickness, transport properties, ther-
mal and electrical properties, and compressibility of the GDL.
The final section sheds light on the GDL modification,
attempted to date, to improve the performance of a URFC.
GDL materials
Hydrogen side GDL material
The most commonly-used CGDL in PEMFCs are carbon paper
(non-woven) and carbon cloth (woven). Carbon felt is also
used as GDL that is non-woven; however, it has different
properties compared to carbon paper [87]. CGDLs can also be
used for the hydrogen side in URFCs and electrolysers. As
metals are prone to hydrogen embrittlement, it is more
practical to use CGDLs for the hydrogen side [88]. The default
GDLs used in PEMFCs are carbon-based materials, which are
mostly in the form of carbon fibre paper (nonwoven) and
carbon cloth (woven). Their porous structure and high
electrical and thermal conductivity are suitable for PEMFC
operating conditions and requirements; moreover, their
production technology is relatively mature that makes the
manufacturing process easier to implement. This type of
GDL is commercially available with different properties and
a wide range of treatments for different operating conditions
[89,90]. Carbon papers are manufactured through
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
impregnation of carbon fibres with a thermoset resin. The
carbon fibres are graphitised at temperatures over 2000  C to
achieve improved electrical conductivity and mechanical
properties. In carbon cloths, as carbon fibres are woven,
there is no need for using a binder. For manufacturing car-
bon cloth, graphitisation occurs after spinning and weaving
of carbon yarns [90]. Detailed manufacturing and processing
methods for carbon fibre cloth and paper can be found in
Ref. [90]. One advantage of CGDLs in stack design is their
compressibility that can compensate for dimensional
changes during the operation due to the effect of pressure
and temperature variation and membrane swelling caused
by hydration [88].
The existing literature is mainly focused on the GDL for the
cathode side of PEMFCs, where water is produced, due to its
significant role in water management.
Oxygen side GDL material
For the oxygen side of URFCs, the rapid corrosion of CGDLs is a
key challenge. In order to address this issue, three different
methods have been used by different researchers. This in-
cludes using corrosion resistive materials, mainly titanium
[57,59,60,91e95]; modification of the CL to inhibit carbon
corrosion [56]; and using protective micro-layer to protect the
GDL [55,62,96e98].
Porous titanium GDLs, in the form of sintered titanium
fibre (Fig. 3a) [57e61,91,99,100] and sintered titanium powder
(Fig. 3b) [93,94], are mostly used in URFCs, similar to PEM
electrolysers [101e105]. Mo et al. [106e108] have used thin
perforated titanium foils to manufacture a customisable GDL
and reduce the cost and cost that can also be investigated for
PEM-URFCs. The reason that titanium-based GDLs are used for
these applications is the high corrosion resistance of titanium
in electrolysis environment. However, the formation of a
highly-electrically resistive titanium oxide can increase
interfacial contact resistance (ICR) and adversely affect the
performance [109e111]. In particular, oxidation of titanium at
the oxygen side is significant due to the presence of active
oxygen species and high overpotential during the electrolysis
operation that results in high contact resistance [110]. In
addition, Ti species can contaminate the MEA resulting in
degradation and performance drop [111]. Pt-coating is one
way to protect the titanium GDL from oxidation and corrosion
[61,111,112], similar to the coating of BPPs made out of tita-
nium [43,44].
While in PEM-URFCs the use of metallic GDLs is limited to
sintered titanium fibres or powder, different types of metallic
GDLs have been used in PEMFCs. This includes perforated
metal foils (e.g. copper [113,114], titanium [115] and stainless
steel [116e121]), metal foams (e.g. NieCr and stainless steel
foam [122], titanium foam [123]), sintered titanium fibre or
powder [110,124,125], stainless steel mesh with a mixture of
water repellent filer and electrically conductive powder
[126,127], and stainless steel fibre [128]. Perforated metal
sheets do not provide an effective distribution of the reactants
as they partially block the CL and the distribution of the re-
actants is unidirectional (through-plane only). Therefore, the
performance is lower than that can be achieved with con-
ventional GDLs [113,114,119e121]. To address this issue, it is
 international journal of hydrogen energy xxx (xxxx) xxx
Fig. 3 e SEM images of sintered titanium fibre (a) and sintered titanium powder (a) GDLs.
tried to cover their surface by a microporous layer (MPL)
[113,119e121] or to connect the micro-holes through micro-
channels in order to provide in-plane reactant distribution
[119e121]. It is worth though to investigate the applicability of
non-precious metal alloys with a protective coating suitable
for electrolysis environment in URFCs to reduce the cost of the
stack.
Some researchers have tried to inhibit the corrosion of
CGDL in URFCs by structural modification of the CL [56] or by
using a protective MPL [55,62,96e98]. Lee and Kim [56]
improved the cyclic performance of a URFC utilising CGDL
by implementing a layered CL to protect the CGDL from
corrosion. As Pt acts as a catalyser for carbon corrosion, they
proposed IrO2/Pt/IrO2 structure for CL so the carbon (GDL) is
not in direct contact with Pt. They also recommended to
minimise the Pt-loading in the oxygen CL to the point that the
FC performance is not compromised [56].
Song et al. [96] developed a protective MPL for a URFC by
using Ti/IrO2 applied on carbon paper. They used IrO2 in order
to catalyse active oxygen species to form oxygen molecules
and prevent the oxidation of Ti and carbon paper. They found
that the FC performance using Ti/IrO2 MPL is on a par with
conventional GDLs while the electrolysis performance is
significantly better. Also, they have reported that the cyclic
performance of the URFC with Ti/IrO2 MPL is stable after 40 h
of continuous operation (20 cycles), whereas the URFC with a
conventional GDL failed to operate after 10 h (5 cycles). A
Similar approach has been implemented by Ma et al. [129] for
the GDL at anode side of a PEM electrolyser. The protective
layer in their experiment was composed of 0.5 mg cm2 Ir
black at the anode mixed with 30 wt% Nafion. They have re-
ported a slight increase in the performance due to the Ir-
coating of the GDL because of the Nafion content; moreover,
the corrosion rate decreased by half compared to an untreated
GDL after 4 h of operation. This highlights the role of Ir in
protecting the CGDL in E-mode. However, still, the long-term
durability needs to be further investigated.
In another study, Chen et al. [62] used TiC and a composite
made out of TiC (80 wt%) and IrTiOx (20 wt%) as MPL and also a
protective layer for CGDL in a URFC. TiC is corrosion resistive;
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
5
however, in E-mode, it is prone to corrosion and carbon is
oxidised and a layer of TiO2 can cover the surface of TiC,
where carbon is corroded. The rapid corrosion of TiC in elec-
trolyser has also been reported by Roca-Ayats et al. [130]. They
used Pt3Ir nanoparticles as bifunctional electrocatalysts and
compared TiC, TiCN, and TiN as the supports for Pt3Ir. They
reported that Pt3Ir/TiC catalyst delivered the worst perfor-
mance and was the least stable one. This poor performance
was attributed to the formation of CO2 and TiO2 [130]. Using a
similar method to Song et al. [96], in order to address this
drawback, Chen et al. [62] used IrTiOx, acting as a catalyser to
recombine oxygen species and prevent carbon and titanium
oxidation. In order to compare and evaluate the performance
and durability of the proposed MPLs, they used a commercial
carbon paper (TGP-H-060) without any protective layer as well
as two other carbon papers, one with TiC and one with TiC/
IrTiOx with two MPLs. By comparing their cyclic performance,
they found that the cell with carbon paper and without any
protective treatment undergoes a rapid degradation and stops
working after the third cycle. The cell with TiC performed
better; however, it also showed noticeable performance
deterioration, lasting only for three more additional cycles. On
the other hand, the cell with TiC/IrTiOx delivered a stable
performance over 15 cycles with a slight performance loss in
FC-mode [62]. Huang et al. [55] have used Ir/TiN as a protective
MPL and have observed a significant improvement in the
URFC performance stability over 20 cycles compared to a
carbon-based MPL. This suggests that the protective layer was
effective in inhibiting the corrosion of the CGDL during the E-
mode.
Sadhasivam et al. [131] have reported that graphitised
carbon (Gr-carbon) obtained by thermal treatment of amor-
phous carbon can be used to form MPL for oxygen-side GDL.
The use of Gr-carbon was reported to improve the perfor-
mance and also reduce the GDL corrosion and surface oxida-
tion. After 20 cycles a high roundtrip energy efficiency of 42.3%
was reported by using Gr-carbon [131]. It is noteworthy that
using Gr-carbon showed improvement in electrical contact
resistance that contributed to the performance enhancement
of the URFC.
6 international journal of hydrogen energy xxx (xxxx) xxx
The use of protective MPL on a CGDL impedes the corrosion
of carbon; however, it does not fully eliminate the corrosion.
Previous studies [55,62,96e98] have been mainly conducted
for a limited number of cycles (i.e. less than 20) that leaves the
long-term durability effect of using MPLs to be still an open
question for further investigation. Therefore, currently,
titanium-based GDLs are the first choice in practical use to
address the durability and further research is needed to
examine the suitability of other materials and protective
methods in long-term applications.
Carbon paper and carbon cloth comparison
As previously mentioned, carbon cloth and carbon paper have
different fabrication methods and hence have different
structures and properties. Therefore, they exhibit different
performance in different operating conditions and cell
designs.
Several studies have compared carbon paper and carbon
cloth properties [132e141] and their impact on the perfor-
mance of PEMFCs in different operating conditions [142e151].
Many researchers have suggested that carbon cloth is superior
to carbon paper in high humidity and/or high current den-
sities (wet conditions) due to having better properties for
water removal [142,143,145,147,151e153] and at lower current
densities carbon paper yields higher performance
[143,147,151]. Wang et al. [147] compared carbon paper and
cloth through experiment as well as a 3D two-phase flow
simulation. They concluded that carbon cloth gives better
performance in high humidity and carbon paper has better
performance at low humidity. Stampino et al. [151] reported
that in lower current densities (i.e. < 800 mA cm-2), carbon
paper results in better performance at different humidity
levels for air (hydrogen was supplied with a relative humidity
of 100% and air with 100%, 80%, and 60% relative humidity).
However, based on their findings, carbon paper suffered from
water management issues at higher current densities. Kowal
et al. [135] by using neutron imaging have shown that
compared to carbon cloth, carbon paper is more prone to
flooding as more water is accumulated under the ribs. Ralph
et al. [142], Frey and Linardy [145] and Sasabe et al. [153] have
concluded that carbon cloth gives better performance at
higher current densities while the performance of carbon
cloth and carbon fibre GDLs are similar at lower current den-
sities. They concluded that liquid water, in the carbon cloth
GDL, is concentrated at the weaves of the fibre bundles (larger
pores), and hence is effectively discharged to the channel. The
oxygen can diffuse through the smaller pores inside the fibre
bundles, which is why the carbon cloth GDL can maintain the
cell voltage under the high current density operations [145].
Contrary to these reports, Sasikumar and Ryu [144] have re-
ported that carbon paper has better performance than carbon
cloth and they have mentioned that because of higher thick-
ness and density of the carbon cloth it faces mass transport
limitations that is significant at high current densities. How-
ever, it should be noted that they have not mentioned the
humidification condition, which plays a significant role in
PEMFC water management. Radhakrishnan and Haridoss [137]
have reported that carbon cloth, due to its structural proper-
ties and higher compressibility, exhibits more intrusion into
the channels, which is more significant when the channel
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width is higher than 1 mm. For wider channel designs, up to
3 mm, they recommended the use of carbon paper over car-
bon cloth.
Moreira et al. [143] investigated the use of a combination of
carbon cloth and carbon paper at anode and cathode sides.
They concluded that carbon cloth is superior at higher current
densities, whereas carbon paper gives slightly better perfor-
mance at lower current densities. They recommended that
using cloth/paper/paper at anode-side (carbon cloth next to
the CL) and carbon cloth at cathode-side improves the cell
performance. However, the tests were carried out using pure
oxygen minimising the diffusion losses. Diffusion losses can
be significant if air is used.
In general, these behaviours are attributed to the structural
differences of carbon cloth and carbon paper. Higher porosity
of carbon cloth has been suggested as a contributing factor for
better performance at higher current densities [142]; however,
it must be noted that carbon cloth is more compressible
compared to carbon paper and the in-situ porosity must be
considered and compared. Carbon paper, due to its highly
tortuous structure compared to carbon cloth, retains more
water, especially under the ribs. Hence, the oxygen concen-
tration is lower in carbon paper compared to carbon cloth,
which is significant in regions under the rib. Therefore, in
fully-wet conditions and high current densities, oxygen con-
centration polarisation has the dominant role and conse-
quently, carbon cloth gives a better performance. On the other
hand, low humidity conditions mean that the membrane
hydration plays a more significant role as its conductivity
decreases by a decrease in its hydration level; therefore, the
membrane's ohmic resistance will be dominant factor. Sub-
sequently, carbon paper, which maintains more moisture,
shows a better performance by keeping the membrane hy-
drated. Wang et al. [147] have also mentioned that carbon
paper has a smoother surface, which makes it more difficult to
remove the water droplets from its surface compared to car-
bon cloth and also water droplets formed on a carbon paper
Table 1 e Performance comparison of carbon paper and
carbon cloth at different conditions.
Condition GDL with better Reasons
performance
High current Carbon cloth
higher porosity
density [142,145]

more efficient water
removal due to
 lower tortuosity
[142,145,147]
 Rough surface [147]
 Dual pore size dis-
tribution [153]
Carbon paper
improved distribution
of reactants

lower density [143]

lower thickness [144]
Low current density Carbon paper
Mitigating membrane
(<800 mA cm2) dehydration
/Low humidity [143,147,151]
 international journal of hydrogen energy xxx (xxxx) xxx
are larger in diameter. The summary of these findings is
presented in Table 1.
GDL properties
Overview
In this section, the main properties of the GDL that affect the
performance of URFC (both in FC and E-modes) are discussed.
The GDL properties determine how it affects the cell perfor-
mance in different operating conditions. Therefore, the
following properties that are shown to affect the URFC per-
formance are discussed in this section: porosity [154,155],
thickness; pores size distribution [60,105]; transport properties
(i.e. diffusivity [156] and permeability [157e159]); thermal
[83,160,161] and electrical [162e167] conductivities; and
compressibility [168e170].
Porosity
GDL porosity and its manufacturing process affect its other
key properties [154,155] such as electrical conductivity [171],
thermal conductivity [172], permeability [172e174], and con-
tact angle [175] of the GDL. Therefore, the porosity of GDL has
an important role in the performance of URFC. In experi-
mental studies [58,59,91,93], a porosity of around 70% is usu-
ally used for GDL in PEM-URFCs. The work done by Hwang
et al. [60] is the only study that has investigated the effect of
GDL porosity on the performance of URFCs by evaluating Ti-
felt GDLs with the porosities of 50% and 75%. They have re-
ported that in FC-mode, lower porosity improves the perfor-
mance in wet conditions by providing lower mass transport
resistance. However, it should be noted that the two samples
had also different pore sizes. The mean pore sizes for 50% and
75% Ti-GDL were 23.3 mm and 45 mm, respectively. This dif-
ference in pore size might also affect the performance; how-
ever, understanding this effect needs further investigation to
deconvolute the effect of these two factors.
Few studies have investigated the effect of GDL porosity in
PEM electrolysers experimentally [105,176e178] and numeri-
cally [176]. Grigoriev et al. [105] have mentioned that higher
porosity GDLs facilitate gas removal but increase the ohmic
losses by increasing the electrical resistance of the GDL and
also the ICR between GDL/CL and GDL/BPP. They have re-
ported that the porosity of GDL in PEM electrolysers should lie
between 30% and 50%. Ito et al. [60,177,178] evaluated 50% and
75% porosities and reported that the porosity did not affect the
electrolyser's performance.
Contrary to the findings by Grigoriev et al. [105] and Ito et al.
[60,177,178], Han et al. [176] reported that higher porosities can
improve the liquid-water saturation through the thickness of
GDL and hence possibly improve the PEMFC performance.
They investigated the liquid water saturation in PEM electro-
lyser GDL by developing a two-phase transport mathematical
model. It should be noted that in their model, the effect of
porosity on electrical conductivity was not considered.
In PEMFCs, higher GDL porosities increase the oxygen mole
fraction at oxygen side and facilitate species transport that
can enhance the performance [165,179,180]. On the other
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7
hand, higher porosities lead to higher ohmic losses as the
electrical resistance increases by porosity [171,181]. Also, a
GDL with higher porosity suffers from inferior mechanical
properties [182,183], which are vital for proper support of the
MEA. Therefore, the optimal porosity is determined by
considering a trade-off between the aforementioned
characteristics.
Similar to the findings by Nabovati et al. [184], Zhan et al.
[65,185] observed higher liquid water content in the GDL as
well as higher effective gas diffusion factors at higher poros-
ities. However, they did not report the effect of porosity on the
performance and they only used a mathematical model to
predict the effect of porosity on liquid water content and gas
diffusion. Nabovati et al. [184] used LBM1 to numerically
analyse a GDL and investigate the effect of GDL porosity,
porosity distribution (heterogeneity), and fibre volume frac-
tion on permeability and tortuosity of the GDL. Their results
showed that by increasing the porosity, tortuosity decreases
while permeability increases (both in-plane and through-
plane). They also found that porosity heterogeneity in-
creases in-plane permeability and decreases the through-
plane permeability. However, they have reported that the ef-
fect of porosity heterogeneity is negligible compared to
porosity and fibre volume fraction. In the case of PTFE coated
GDLs, they reported that increasing the fraction of PTFE and
binder and decreasing the fraction of fibres resulted in an in-
crease in permeability and tortuosity [184].
Larbi et al. [165], by developing a numerical simulation,
showed that the higher the GDL porosity the higher the mole
fraction of oxygen, resulting in the electrochemical reaction
improvement. Higher porosity results in higher limiting cur-
rent density as mass transport limitations are more pro-
nounced at higher current densities. They found that when
porosity is lower, relatively higher amount of the total current
is generated under the channel [165]; this can be explained by
the fact that when porosity decreases, the in-plane gas
permeability will also decrease and therefore the oxygen mole
fraction under the ribs will be much lower than that of
available under the channels. Therefore, hot spots can be
developed inside the MEA resulting in the membrane dehy-
dration (reduction in proton conductivity) and degradation.
This leads to a decrease in the proton conductivity. However,
it must be considered that higher porosity means higher
electrical and thermal resistance that both have negative
impacts on the performance of the cell [165].
By using a CFD simulation, Karpenko-Jereb et al. [186] also
reported a significant increase in the in-plane transport of
reactant gases and the product water in the GDL by an in-
crease in the GDL porosity from 78% to 97.5%. However, their
simulation showed that this improvement in species trans-
port results in membrane dehydration (i.e. increased ohmic
resistance) and hence a significant performance drop (70%
drop in limiting current density).
The findings reported by different research groups indi-
cated that GDL porosity gradient improves water manage-
ment and effective transfer of reactant gases [65,185,187,188]
and uniformity of the current distribution across the cell area
[188e190] in PEMFCs. Therefore, it is worthwhile to investigate
1
Lattice Boltzman Method.
8 international journal of hydrogen energy xxx (xxxx) xxx
graded porosity GDLs in URFCs for opportunities to improve
the performance and durability. Considering the difficulty of
producing graded porosity in CGDLs used in PEMFCs, GDL
porosity gradient is mostly investigated numerically. Howev-
er, using metallic GDLs in PEM-URFCs and electrolysers pro-
vides the opportunity to utilise powder metallurgy and
develop functionally graded materials (FGM) [191,192]. Ti-
based FGMs are currently being used in biomedical [193,194]
and precision filtering [195] applications. Qian and Froes
[196] have covered a wide range of different titanium powder
sintering methods in details. These methods can offer op-
portunities for experimental investigation of using graded
porosity GDL in URFCs and its impact on the performance of
both FC and E-modes.
Thickness
One of the factors in designing and selection of GDLs is the
thickness that can affect water management and reactants
delivery to the active area. A trade-off between performance,
cost, and durability determines the optimal thickness of the
GDL. Generally, the following points can be considered based
on the findings from published literature (considering MPL is
applied):

The thicker the GDL, the longer the length of the diffusion
paths (higher tortuosity) and lower through-plane perme-
ability [72,197,198].

Thicker GDLs are more prone to water flooding in FC-mode
[197,199].

Thicker GDLs have higher thermal and electrical re-
sistances [198,200].

Thinner GDLs are suitable for cells operating under high
humidity and/or high current densities whereas thicker
GDLs are more effective for dry conditions and/or low
current densities to keep the membrane hydrated [197].

GDL thickness can affect its mechanical properties and
hence its support for the membrane, which is of great
importance in high-pressure PEM water electrolysis.
In the case of URFCs, usually, Ti-foams or felts with a
thickness between 250 mm and 1000 mm have been used in
different experiments [57,59e61,91,93,201]. The effect of the
GDL thickness on the performance of URFCs has not been
investigated in the published research papers. Moreover, the
limited studies that investigated the influence of the GDL
thickness on the performance PEMFCs have mainly focused
on carbon paper or carbon cloth [67,202e207]. Hence in this
section, the findings from the research on PEM electrolysers
and FCs will be discussed that can help with the selection of
GDL thickness for PEM-URFCs.
For electrolysers, Han et al. [176,200,208] investigated
numerically [176,208] and experimentally [200] the effect of
GDL thickness on the performance of a PEM electrolyser. Their
findings indicated that the electrolyser performance improves
by a decrease in the GDL thickness. They suggested that
thicker GDLs increase diffusion and ohmic losses. Contrary to
the findings of Han et al. [176,200,208] and almost all the
findings of other similar studies on GDL thickness, Siracusano
et al. [209] reported a lower ohmic loss for thicker GDLs. The
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specific resistance of the cells with the thick and thin GDLs
were 0.7 U cm2 and 1.7 U cm2, respectively. It can be observed
that the effect of GDL thickness is very significant and the
thinner GDL has increased the total resistance by almost
143%. However, in PEMFCs or electrolysers, usually, it is not
expected that the effect of GDL resistance to be as high as this.
They have compared the two GDLs by applying 15 kg cm2 of
assembly pressure. However, it was not reported that how the
pressure was measured and whether it was the effective
pressure on the MEA. One possible explanation for higher
electrical resistance using the thinner GDL is that possibly the
same gasket was used in both setups (i.e. the thickness of the
gasket has not been changed according to the GDL thickness)
and hence the thinner GDL underwent lower compression
compared to the thicker GDL (i.e. when the same stack as-
sembly load was applied). Hence the contact resistance could
be much higher when the thinner GDL was used due to lower
effective compressive load on the GDL.
In PEMFCs, the research on GDL is mostly carried out when
MPL is applied to the main substrate [72,197,198,210]. In
PEMFCs, thicker GDLs have higher tortuosity and are more
prone to flooding at high humidity conditions or high current
densities [197]; a thinner GDL can effectively remove the water
from the CL to the flow channels and provide a more stable
performance [197,198]. Due to the same reason, thicker GDLs
are favourable for use in lower current densities or low hu-
midity conditions as they can prevent membrane dehydra-
tion. Thicker GDLs have lower through-plane gas permeability
[72,198] while they have higher in-plane gas permeability [72].
Therefore, for interdigitated flow fields, thicker GDLs are
suitable as they can provide higher in-plane permeability; on
the other hand, thinner GDLs are suitable for parallel channel
flow fields. In parallel channels, high in-plane gas perme-
ability can encourage blockage of the channels by facilitating
gas flow bypass (i.e. the accumulated liquid water in the flow
channels is not removed effectively) [210]. However, it is
important to note that a thicker GDL also increases the
diffusion pathway [197] and hence an optimum thickness is
required to achieve the maximum performance in a range of
operating conditions and the flow-field design. Lin et al. [67]
reported that when GDLs without MPL were used in PEMFC,
water accumulation had a more significant impact on thinner
GDLs as they have lower pore volume compared to thicker
GDLs and hence when liquid water fills the pores, less pore
volume remains empty for gas transport.
The effects of thickness on other properties of GDLs
including droplets contact angles and breakthrough pressure
in GDL have also been investigated. Mortazavi and Tajiri
[204,205] reported that thickness has no effect on the droplet
contact angle and the mean pore diameter of GDL. When the
GDL thickness increases, the effect of PTFE loading decreases
and eventually, the treated and untreated GDLs will have the
same level of water saturation [211]. The breakthrough pres-
sure in GDL increases by increasing the GDL thickness [212].
As the thickness increases, flow path length also increases,
which means more pores must be filled with liquid water until
the liquid water reaches the GDL surface. Also, for thicker
GDLs, there is a higher chance for small pores, which have
higher capillary pressure, to be in the path of the liquid water
[205,206,212]. Fig. 4 illustrates the effect of GDL thickness on
 international journal of hydrogen energy xxx (xxxx) xxx
Fig. 4 e Impact of GDL thickness on breakthrough pressure
for different PTFE loading [212].
the breakthrough pressure with different PTFE loading of the
GDL.
Pore size distribution
Studies conducted on the effect of pore size of GDL in URFCs
[60,105], and metallic GDLs, in general, are very limited.
Hwang et al. [60] investigated the effects of GDL properties on
URFC performance. They have considered the effect of GDL
fibre diameter in their experiments on the performance of a
URFC. While they did not report an optimal pore size for Ti-
GDL, they reported that using larger fibre diameter (i.e.
80 mm in their experiments) help improve the roundtrip en-
ergy efficiency of the URFC when the reactants are fed at high
relative humidity (i.e. humidification temperature of 75  C and
cell temperature of 80  C) compared to a GDL with lower fibre
diameter (i.e. 20 mm). The GDL sample with larger fibre
diameter has significantly larger pore size distribution. They
mentioned that a non-uniform pore size distribution im-
proves the water management and hence the performance of
the URFC in FC-mode.
For electrolysers, a pore diameter of around 12e13 mm was
reported to be the optimal value [105,177]. Grigoriev et al. [105]
investigated the microstructure of sintered titanium powder
used in a PEM electrolyser. At atmospheric pressure, they
found that mean pores diameter of 12e13 mm gave the best
performance, which can be achieved by using titanium pow-
ders in the range of 50e70 mm. The capillary effect gets more
significant as the pore size decreases. In PEM electrolysers,
Grigoriev et al. [105] showed that the capillary effect is not
significant when the pores size is larger than 10 mm and
consequently there is an slight increase in the equilibrium
voltage. On the other hand, they reported that using larger
titanium particles results in higher ohmic losses and less
homogeneous current distribution that can lead to hot-spot
formation that damages the membrane permanently. To
reduce these ohmic losses, they found that the gap between
the particles in touch with the catalyst layer must be reduced.
This can be achieved by using smaller particles. They sug-
gested that these findings are applicable to GDLs in URFCs.
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9
Similarly, Ito et al. [177,178] investigated the effect of GDL pore
size in PEM electrolysers. They reported that for pore sizes
greater than 10 mm, the electrolyser performance increases by
decreasing the pore size [177]. The concentration over-
potential increases by increasing the mean pore diameter of
the oxygen side GDL. This is because larger oxygen bubbles
emerge from larger pores that can form long slugs deterring
the water supply to the active area [177]. Improved contact
between GDL and CL reduces both ICR and the activation
overpotential [178].
Han et al. [176] numerically investigated the effect of GDL
pore size in PEM electrolysers and the findings were not in
agreement with those reported by Grigoriev et al. [105] and Ito
et al. [177,178], They considered pore sizes between 35 mm and
95 mm and found that liquid saturation in GDL increases by the
increase in pore size [176]. They also concluded that larger
pores might help improve the PEM electrolyser performance.
In addition, the liquid saturation through the GDL thickness
decreases for larger pore diameters, indicating that more
liquid water exists in thicker GDLs. It should be noted that
they only introduced the effect of pore size on the perme-
ability of the GDL and other effects such as capillary effects
and ICR were neglected.
It has been suggested that bimodal pore size distribution
enhances the species transport and improves the perfor-
mance in PEMFCs [138,153,213]: few in-plane and through-
plane large pores should exist in the GDL for collection and
removal of liquid water through the GDL and the rest of the
GDL consist of small hydrophobic pores (that should be ideally
as small as possible) that are not filled with water and provide
a passage for reactant gases [138,213]. Moderate pore size
gradient is also shown to be beneficial for water management
and removal of excess product water from the cell, resulting in
improved fuel cell performance [214,215].
Pore size, or particle/fibre diameter, can affect some of GDL
properties such as mechanical strength and permeability
[216,217]. In metallic GDLs, the pore size can affect their me-
chanical strength [216]. For sintered titanium powder, smaller
pore size distributions result in a lower elastic modulus [217].
This can affect the optimal design of the whole stack and
especially gasket design and assembly pressure. However, for
electrical [218] and thermal conductivity [219] and diffusivity,
no obvious relationship with pore size has been reported
when the pore size is sufficiently small compared to the GDL
dimensions.
One drawback of CGDLs is that their properties are not
repeatable and properties of the same product are not very
consistent and usually vary significantly from one to another
[220]. The use of metallic GDLs gives more control over
different physical properties of GDL such as porosity and pore
size distribution compared to CGDLs [216]. Therefore, it pro-
vides opportunities for a detailed investigation on the role of
these parameters on URFC performance in both FC and E-
modes by keeping other parameters reasonably constant.
Transport properties
Diffusivity
The GDL effective diffusivity is a measure of how reactants/
products in form of gas/vapour can quickly travel through the
10 international journal of hydrogen energy xxx (xxxx) xxx
porous structure of the GDL. GDL should effectively provide
the transport pathways for reactants and products. Diffusion
is considered to be the main transport mode in the porous
media used in PEMFCs [141]. In other words, diffusion in GDLs
is an important deterministic parameter in FC-mode opera-
tion, especially at high current densities, for effective reactant
supply to the active area. As a result, in order to improve the
FC-mode efficiency and performance by reducing the mass
transport limitations, the diffusivity of GDLs should be care-
fully considered [221e223].
Due to the presence of the solid phase of the GDL and liquid
water in the pores of a partially-saturated GDL, the effective
diffusion coefficient is not the same as the diffusion coeffi-
cient of oxygen or hydrogen in a gas mixture environment in
the absence of solid or liquid phases [156]. The widely used
method for measurement of the GDL effective Diffusivity, Deff,
is Loschmidt cell [224e226]. Rashapov et al. [222] have devel-
oped a new and simple method to measure the in-plane
diffusivity of thin porous materials. In their method, the
porous sample is initially purged by nitrogen. Oxygen, from
air, diffuses into the sample. At a specific location, over time,
the concentration of oxygen is measured in the sample. Then
the results are fitted to the analytical solution of 1-D transient
Fick's law of diffusion. Yang et al. [227] also proposed a new
method for measuring the effective diffusion coefficient in
porous media by implementing an air-breathing PEMFC to
create an oxygen concentration gradient. They claimed that
this method provides a more reliable measurement of diffu-
sion coefficient for non-wetting GDLs [227]. By using a sample
holder, the GDL (porous sample) is placed in the cathode BPP.
The oxygen concentration difference across the GDL is
correlated with the PEMFC voltage difference with and
without the inserted GDL sample. The effective diffusion co-
efficients can be obtained from the oxygen concentration
variation across the GDL sample for a specific oxygen flux
[227]. Chevalier et al. [228] have recently introduced a method
to measure the in-situ effective diffusivity of partially satu-
rated GDLs and MPLs. They combined ex-situ measurement of
GDL porosity distributions by X-ray tomography and in-situ
measurement of liquid water thicknesses by synchrotron X-
ray radiography to obtain the profiles of through-plane liquid
water saturation. The effective diffusivity of the partially
saturated GDL and MPL were determined by analysing Elec-
trochemical Impedance Spectroscopy (EIS) measurements
with the developed 1-D model of FC impedance [228].
Bruggeman's approximation [229,230] is commonly used
for estimating the GDLs' effective diffusivity [231,232]; how-
ever, it is reported by some researchers [225,233,234] that it
overestimates the effective diffusivity of CGDLs; at higher
current densities and lower porosity ranges, this can result in
underestimating the species transport limitations in the GDL
[225]. In general, the relation between Deff and the bulk diffu-
sivity, Db, for an unsaturated porous material can be written as
Deff =Db ¼ f ðεÞ, where f ðεÞ is a function of the GDL porosity, ε.
Other researchers have proposed different formulae to esti-
mate the effective diffusion coefficient, presented in Table 2.
The parameters in the model proposed by Tomadakis &
Sotirchos [236] for different structures and flow directions can
be found in Table 3. In this equation, εp is the percolation
threshold.
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Hossain et al. [242] developed a single-phase 3-D model for
a PEMFC to compare different GDL effective diffusivity
models. By comparing several models proposed by other re-
searchers [235,236,238,240], they concluded that by using
Tomadakis and Sotirchos [236] equation in their model, the
calculated cell voltage was the closest to the experimental
values.
GDL Saturation has a negative impact on gas diffusion as
some of the pores will be occupied by liquid water resulting in
the blockage of diffusion pathways. The effective diffusivity
for saturated GDLs can be expressed as Deff =Db ¼ f ðεÞgðSÞ,
where S is the GDL liquid water saturation (i.e. the ratio of
water volume to the total pore volume) and gðSÞ is the nor-
malised function of liquid saturation. PTFE-coating provides a
better pathway for gas diffusion that increases g(S) [243].
Different proposed models for diffusivity in saturated porous
structures are presented in Table 4.
The results of the numerical simulation conducted by Wu
et al. [241] showed that the oxygen effective diffusivity in-
creases with decreasing heterogeneity and increasing pore
connectivity. It was also reported that the ordered distribution
of fibres increases the diffusivity compared to a random dis-
tribution [79].
The diffusion of dry GDLs decreases by the binders used in
CGDLs [79,230], PTFE-coating of the GDL [222,225,230,233,241],
and the addition of MPL, especially with an increase in the
penetration of the MPL into the GDL substrate [224,233]. In a
dry GDL, the effective diffusion coefficient is decreased
significantly by an increase in PTFE loading of the GDL that can
be a sign of porosity and pore size reduction [224,233] and an
increase in tortuosity [233]. However, in partially-saturated
GDLs, PTFE coating enhances the diffusion by keeping some
of the pores free of water [223]. In the absence of MPL, for
carbon paper GDLs, it was reported that the effective diffusion
coefficient is not affected by the operating temperature [225]
and the thickness [224].
Permeability
The permeability of GDL can affect the performance of the
PEMFC in serpentine and interdigitated flow field designs due
to the pressure difference between adjacent channels [157]. It
was shown that higher permeability increases the limiting
current density [157]. Also, it has been shown that higher
permeability can improve the performance in straight parallel
channels at current densities higher than 0.5 A cm2 [158,159].
On the other hand, in parallel channels, the permeability of
the GDL can affect the water transport in the flow channels
[81,139,168]; in PEMFCs with parallel flow channel design,
water emerges into the gas flow channel from the GDL and
forms droplets. The droplets grow into slugs that can block the
flow channel. Once the slugs are formed, gas will bypass the
slugs by flowing through the porous GDL if the pressure drop
through the GDL is lower than the pressure required to
remove the slug from the channel that can happen when the
GDL permeability is high enough. The slugs continue to grow
until the differential pressure for gas flow through the GDL
equals the differential pressure required to move the slugs
[81,168].
It is suggested that the high isotropic permeability or a
combination of high in-plane and low through-plane
 international journal of hydrogen energy xxx (xxxx) xxx 11

Table 2 e Mathematical models for effective diffusivity in non-saturated porous media.fðεÞ

Model Note Reference
Deff Spherical particles [231]
¼ ε1:5
Db
Deff 2ε Spherical particles [235]
¼
Db 3ε


Deff ε  εp f Random fibres [236]
¼ε
Db 1  εp
Deff ε Aligned fibres [237]
¼
Db 2ε
Deff Spherical particles 0  ε 0.65 [238]
¼ 1  ð1  εÞ0:46 *
Db
 
Deff 3ð1  εÞ Spherical particles [239]
¼ 1
Db 3ε
Deff ðε  0:11Þ0:9 Spherical particles [240]
¼
Db ð1  0:11Þ0:9
 
Deff 3ð1  εÞ 3-D random fibres through-plane 0.33  ε 1 [231]
¼ 1  2:76ε coshð3ε  1:92Þ
Db 3ε
 
Deff 3ð1  εÞ 3-D random fibres in-plane
¼ 1  1:72ε coshð2:07ε  2:11Þ
Db 3ε
Deff ε 1-D random fibres [79]
¼
Db 2:7  1:7ε


Deff ε 3:7  1:7ε 4 2-D random fibres
¼ þ
Db 4 2:7  1:7ε 3:7  1:7ε


Deff ε 4:7  1:7ε 9 3-D random fibres
¼ þ
Db 6 2:7  1:7ε 6:4  3:4ε
Deff 3-D random fibres [241]
¼ eðε1Þ=ð0:2220:161Cp Þ *a
Db
In these equations: Deff is effective diffusivity; Db is bulk diffusivity, ε is the GDL porosity, and Cp is the PTFE content by weight.
a
The effect of pore blockage is not presented here. For further details please refer to Mezedur & Kaviany [238].

permeability results in higher performance of a PEMFC

[159,168]. The FC performance significantly deteriorates with
Table 3 e The dimensionless constants for Deff formula
low in-plane and high through-plane permeability of GDL
proposed by Tomadakis & Sotirchos [236].
[159,168]. It has also been shown that the GDL permeability is
Structure Flow direction εp f
not affected by hydrophobic coating [245].
1-D Parallel to the fibres 0 0 Several models are available for prediction of permeability
Perpendicular to the fibres 0.33 0.707 in porous media. Some of these models that are relevant to the
2-D Parallel to the fibre planes 0.11 0.521
porous structure of GDLs used in PEMFCs are presented in
Perpendicular to the fibres planes 0.11 0.785
Table 5. The constants used in the Tomadakis and Sotirchos
3-D All directions 0.037 0.661
permeability model are presented in Table 6. Also, it should be

Table 4 e Mathematical models for effective diffusivity in saturated porous media.

Model Note Reference

 Nam & Kaviany [244]
Deff ε  0:11 0:785 Spherical particles
¼ε ð1  SÞ2
Db 1  0:11
Deff 3ð1  fg Þ Spherical particles Das et al. [239]
¼ 1þ
Db 3Db
 fg
3ð1  fl ÞDl
Db  Dl 
fl  3ð1  fg Þ
Deff Random fibres (No PTFE) Hwang & Weber [243]
¼ ε3:6 ð1  SÞ3
Db
  
Deff lnðSÞ þ a PTFE coated random fibres
¼ εm  0:5 1 þ erf  *a
Db b
ðε  0:11Þ0:9 ðð1  SÞ  0:11Þ0:9 Spherical particles Dawes et al. [240]
f ðεÞ ¼ 0:9

ð1  0:11Þ ð1  0:11Þ0:9

In these equations: S is GDL saturation; Deff is effective diffusivity; Db is bulk diffusivity, ε is the GDL porosity, and Cp is the PTFE content by
weight; fg and fl are the volume fractions of gas phase and liquid water in the porous media, respectively.
a
The value of m, a, and b depends on the porous media and are obtained through curve fitting.

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12 international journal of hydrogen energy xxx (xxxx) xxx

Table 5 e Models for permeability in fibrous porous media.

Model Note Reference
r2 ε 3 kCK is the CarmaneKozeny constant which depends on the type KozenyeCarman (KC) model
K ¼
4kCK ð1  εÞ2 of media and is used as a fitting parameter using experimental
data
ε ðε  εp Þðaþ2Þ r2 a and 3p are constants, which depend on the sample fibre Tomadakis and Sotirchos (TS) [247]
K ¼ arrangement (aligned in 1-D, random in 2D or 3D) and on the
8ðlnεÞ ð1  εp Þa ½ða þ 1Þε  εp 2
2

direction of flow relative to the planes of the fibres, normal or

parallel for 1-D and 2D and all directions for 3D. The values
of a and 3 p for different conditions are presented in Table 6.
ε4:3 2 through-plane permeability in random fibre (idealised carbon Van Doormaal and Pharoah [174]
K ¼ 0:28 r ; 0:6  ε  0:8
1ε paper structure)
ε3:6 2 in-plane permeability in random fibre (idealised carbon paper
K ¼ 0:26 r ; 0:6  ε  0:8
1ε structure)
rffiffiffiffiffiffiffiffiffiffiffiffiffi !C2 εc is the percolation threshold. C1 and C2 are related to the Nabovati et al. [173]
1  εc
K ¼ C1 1 r2 geometry of the network. By curve fitting they have obtained
1ε
0.0743, 0.491, and 2.31 for εc, C1 and C2, respectively.

*r is fibre radius and df is the fibre diameter in all equations.

**The value of m, a, and b depends on the porous media as is obtained through curve fitting.

durability that need to be determined for each specific cell

Table 6 e Constants used in the Tomadakis and Sotirchos
design and operating conditions [161]. GDLs with lower ther-
model for permeability.
mal conductivity (i.e. 0.3 W m1 K1 [161]) get less saturated by
Structure Flow direction 3p a
liquid water at high current densities and maintain the oxy-
1-D Parallel 0 0 gen transport resistance at lower levels, this is while the
Normal 0.33 0.707 membrane remains at a higher temperature and lower water
2-D Parallel 0.11 0.521
content that leads to lower proton conductivity. On the other
Normal 0.11 0.785
3-D All directions 0.037 0.661
hand, when GDLs with higher thermal conductivity (i.e.
1.4 W m1 K1 [161]) are used, the membrane temperature
stays at a lower level and its hydration level and hence proton
considered that The addition of MPL reduces the GDL conductivity are higher; however, the GDL can be saturated
permeability and the reduction depends on the amount of with liquid water and hence oxygen transport is negatively
carbon loading and the PTFE content [246]. affected [83,161]. By using GDLs with higher thermal conduc-
tivities the cell temperature settles at a lower level that can
Thermal properties result in increasing the liquid water saturation inside the GDL
[83]. Moreover, GDLs with higher thermal conductivities can
The thermal conductivity of GDL can play an important role in help achieve a more uniform temperature across the cell [83].
water management of PEMFCs [83,160,161]. A balanced ther- Numerical simulation has shown that such uniformity in-
mal conductivity is required for optimal cell performance and creases the current density of PEMFCs [83]. The research

Table 7 e Thermal conductivity models for GDL.

Model Note Reference

keff [264]
max ¼ εkf þ ð1  εÞks
" #1
[265]
ð1  εÞ ε
keff
min ¼ þ
ks kf

ε ð1εÞ
keff
intermed ¼ kf ks

8  
> 0:008 3ε Fibrous media e developed for GDL in PEMFCs [266]
>
keff < 1  0:963ð1  εÞ
> exp½0:881ð1  εÞ
3  ð1  εÞ
through  plane
¼  
ks >
> 3ε
>
: 1  0:977ð1  εÞ0:009 exp½0:344ð1  εÞ in  plane
3  ð1  εÞ
3εks ðkf  ks Þ 3ð1  εÞkf ðks  kf Þ [267]
ks þ  keff  kf þ
3ks þ ð1  εÞðkf  ks Þ 3kf þ εðks  kf Þ
1 Cellular solids [268]
keff ¼ ½ð1  εÞ þ 2ð1  εÞ2=3 ks þ εkf
3
In these equation, keff is the effective thermal conductivity; ks and kf are the thermal conductivity of solid phase and fluid phase, respectively.

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 international journal of hydrogen energy xxx (xxxx) xxx
conducted by Alhazmi et al. [83] showed that in-plane thermal
conductivity had a greater impact on the temperature gradi-
ents across the cell compared to the through-plane thermal
conductivity. However, still, both in-plane and through-plane
thermal conductivities play a role in achieving a uniform
temperature across the cell. Using GDLs with isotropic ther-
mal conductivity results in more uniform current density
distribution and lower temperature gradients compared to
anisotropic GDLs [248].
Compression is another factor that was found to affect the
thermal conductivity of GDLs. It is reported that the thermal
conductivity of GDLs increases by compression [249e256].
This is mainly due to the reduction of porosity of the GDL and
better contact between the fibres. By contrast, Nitta et al. [257]
observed no relation between compression of GDLs and their
thermal conductivity; their measured values of thermal con-
ductivity for CGDL (1.18 ± 0.11 Wm1K1), was almost three to
six times higher than what had been reported by other groups.
It is noteworthy that the range of thermal conductivities of
CGDLs has been mainly reported to between 0.2 and
0.6 Wm1K1 [249e254,258]. The guarded hot-plate method is
the main method used for the measurement of thermal con-
ductivity of GDLs [80,249,256,259e261]. Several theoretical
models have been proposed for thermal conductivity of
porous materials and a selected number of them that are
specifically applicable to GDLs are presented in Table 7.
The thermal contact resistance between the GDL and BPP
decreases nonlinearly with increasing compression pressure
[249e257]. This is attributed to the increase in actual contact
area at the interface as compression pressure increases. The
thermal bulk resistance of the GDL is comparable to the
thermal contact resistance between the GDL and graphite (the
common material for BPP in PEMFCs), suggesting both bulk
and interfacial thermal contact resistance of the GDL should
be considered in modelling studies [249,256,257].
Introducing PTFE and MPL increases the thermal contact
resistance between the GDL and BPP, especially at higher
loadings [249,256,262]. As the porosity of the MPL increases,
the overall thermal conductivity decreases [263]. As a result,
the presence of MPL increases the temperature at the
Fig. 5 e The effect of GDL porosity on the performance of
PEMFC [162].
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13
interface of GDL and CL and hence more water is removed in
the form of vapour [160,262]. Load cycling reduces the total
thermal resistance of BPP-GDL, including bulk and contact
resistances [249].
Sadeghifar et al. [255] have proposed an analytical model
for prediction of thermal contact resistance between fibrous
porous media and flat surfaces applicable to PEMFCs. For
compressions of over 2 bar, their model accurately represents
the experimentally-measured values.
The thermal conductivity of metallic GDLs and their ther-
mal contact resistance has not been reported in the literature;
more importantly, its effect on the performance and water
management has not been investigated. Using different
porous metals gives the opportunity of experimentally
investigating the effect of thermal conductivity of GDL on the
URFC performance that is also applicable to PEMFCs.
Electrical properties
The GDL serves as an electrical conductor between the cata-
lyst layer and the BPP. Therefore, the materials used for GDL
must have good electrical conductivity. Also, the GDL material
should be chemically stable to avoid highly-resistive oxide
layer formation, which is detrimental to electrical conduc-
tivity and translates into performance losses. The electrical
resistance of a GDL increases by increasing its porosity;
however, in PEMFCs, higher porosities are always favourable
for better delivery of reactants to the active area, especially at
higher current densities [162e167]. Therefore, the optimal
porosity is a trade-off between the electrical conductivity and
the species transport properties. The theoretical simulation
conducted by Lin et al. [162] have shown (Fig. 5) that an
optimal porosity for the GDL can be determined by consid-
ering the above-mentioned factors, while parameters such as
thickness and pore size were kept constant in their model.
Metallic GDLs have lower bulk electrical resistance than
CGDLs; however, they are prone to developing an oxide layer,
which lowers the electrical conductivity and negatively af-
fects the electrical contact resistance. It is noteworthy that the
main component of the electrical resistance of GDL and BPP is
the contact resistance between GDL/BPPs and GDL/CL; the
bulk electrical resistance of these components usually ac-
count for less than 10% of the total electrical resistance of the
GDL/BPP combination [269]. Similar to thermal contact resis-
tance the electrical contact resistance is also directly related
to the assembly pressure (i.e. higher assembly pressure re-
sults in lower electrical contact resistance and hence lower
ohmic losses) [270].
Most of the studies on GDLs electrical properties have been
carried out on CGDLs [128,154,271e277]. The contact resis-
tance of metallic GDLs has been studied in a few published
papers, e.g. Refs. [110,128]. Hottinen et al. [110] compared the
sintered titanium GDL with carbon paper. Their results indi-
cated that in comparison with carbon paper, Ti-GDL results in
a higher cell's overall electrical resistance. They reported that
the cell resistance was reduced by almost half by Pt-coating of
the Ti-GLDs. However, the Pt-coated Ti-GDLs exhibited higher
resistance compared to carbon paper. Yi et al. [128] investi-
gated the Sintered Stainless Steel (SS) fibre as GDL in PEMFCs.
They reported that the in-plane and through-plane electrical
14 international journal of hydrogen energy xxx (xxxx) xxx
conductivity of SS-GDL is higher than of a carbon paper. The
main reasons are that the bulk conductivity of SS is higher
than graphite and also the SS fibres are sintered and therefore,
they are welded together at contact points and hence have
better conductivity [128]. They coated the SS-GDLs by amor-
phous carbon to improve the corrosion resistance and lower
the electrical contact resistance. The contact resistance of
amorphous-carbon-coated SS-GDLs was slightly lower than
carbon paper whereas the electrical contact resistance of base
SS-GDL was considerably higher than that of the carbon paper
that is in line with the findings of Hottinen et al. [110].
The contact resistance is usually measured through ex-situ
experiments. The method developed by Davies et al. [278] has
widely been used by different researchers [128,154,271e277].
One shortcoming of this method is that usually the bulk
resistance of materials is neglected compared to the contact
resistance or it is estimated based on the bulk properties of the
material. To address this limitation, based on the technique
developed by Davies et al. [278], Okel et al. [279] developed a
method to simultaneously measure and separate the contact
and bulk electrical resistances of different PEMFC compo-
nents, including GDL and BPP. Similar attempts have been
made by other researchers [269,280]. Some researchers have
tried to measure the in-situ contact resistance between
different components in PEMFCs [281]. Ismail et al. [281]
measured the electrical contact resistance between the GDL
and graphite BPP in an assembled PEMFC. They reported that
for a GDL without MPL, the initial thickness of the carbon GDL
has a positive effect on the contact resistance (i.e. the higher
the thickness the lower the contact resistance) while higher
amounts of PTFE loading increase the contact resistance.
However, it should be considered that the effect of thickness
of contact resistance reported by Ismail et al. [281] is most
probably to using gasket with similar thickness for GDLs with
varying thickness. This will result in higher compression of
the thicker GDL and hence lower electrical contact resistance.
GDLs, due to their anisotropic structure, have different in-
plane and through-plane properties [282,283]. As the fibres
orientation is mainly in-plane, the properties such as elec-
trical and thermal conductivities are usually higher for in-
plane direction compared to through-plane direction [283].
Hydrophobisation of GDL (e.g. PTFE-coating) is shown to not
noticeably affect the GDL conductivity in the in-plane direc-
tion as PTFE-coating does not alter the carbon fibres structure
in the GDL [273]. On the other hand, the electrical contact
resistance, the major factor affecting the overall electrical
Fig. 6 e GDL samples under 2 MPa pressure: a) Ti-felt GDL;
b) ELAT carbon-cloth GDL.
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conductivity in the through-plane direction, is reported to
increase by an increase in PTFE loading [154,273].
Higier and Liu [284] experimentally measured the electrical
resistance under the channels and the ribs. They found that
electrical resistance under the channels, where the GDL is not
compressed by the BPP, is considerably greater than that of
under the ribs, where the GDL is directly compressed by the
BPP, for wide channels (2 mm). On the other hand, for nar-
row channels (1 mm), the electrical resistance in both re-
gions, was reported to have no significant difference [284]. The
lack of compression was reported as the main contributor to
the increased electrical resistance under the channels
resulting in increased contact resistance between the GDL and
CL. Higier and Liu [284] argued that this increase in contacts
resistance under the channels resulted in lower current den-
sity in these areas.
GDL compressibility and stack assembly
The optimal assembly pressure of the stack is a trade-off be-
tween having a low electrical contact resistance and effective
reactants and products transport [270,285e287]. Also, the
applied assembly pressure should be limited to avoid
damaging the components, especially the MEA [270,288]. The
contact resistance makes up the majority of the total electrical
resistance in the stack, which is decreased by an increase in
the assembly pressure [154,269e271,274,277]. As CGDLs are
compressible, under the ribs, their thickness and porosity
reduces and hence the reactants and products transport is
negatively affected [168,169,287,289]; moreover, excessive as-
sembly pressures can cause the CGDL to intrude into the flow
channels hindering the adequate supply of reactants; this
factor needs to be considered in determining the assembly
pressure. For CGDLs, it is shown that thicker GDLs are more
tolerant to a higher level of thickness reduction under
compression for achieving optimum performance in com-
parison with CGDLs with lower thickness. The effect of as-
sembly pressure on CGDLs with lower bulk density is more
significant [170]. CGDLs with lower bulk density require a
higher level of compression (deformation) to achieve opti-
mum performance [170].
One of the main differences between sintered titanium
GDLs, the commonly used GDL in URFCs, and CGDLs is their
compressibility. CGDLs, such as carbon paper, undergo sig-
nificant thickness changes under compression (Fig. 6a). On the
other hand, Ti-based GDLs are relatively rigid and do not show
noticeable deformation under the range of assembly pressure
of URFCs (Fig. 6b). Another factor that should be considered is
the effect of temperature on the CGDL compressibility [290]; at
higher temperatures, the CGDL shows less resistance against
compression and undergoes larger deformation [290]. The
compressive strength on Ti-based GDL is expected to be
affected to a lesser degree by temperature, however, experi-
mental studies are required to clarify the effect of temperature
on mechanical properties of metallic GDLs used in URFCs and
electrolysers.
However, still, there is a limit for the compressive load that
can be applied to Ti-based GDLs and excessive assembly
pressures can permanently deform them. This factor can
affect some aspects of the URFC stack design and assembly
 international journal of hydrogen energy xxx (xxxx) xxx
that have not been addressed in the literature. One advantage
of CGDLs in stack design is their compressibility, which can
compensate for dimensional changes during the operation due
to the effect of pressure and temperature variations and the
membrane swelling caused by hydration [88]. When a more
rigid GDL, such as sintered titanium fibres, is used in URFCs,
these dimensional variations should be addressed through
more sophisticated designs to ensure a uniform compression
during the operation; a summary of different stack assembly
methods can be found in the paper published by Millichamp
et al. [291]. Also, the gasket selection is affected by the change
in GDL compressibility and should be considered in the stack
design [292]. The mechanical properties of sintered titanium
can be altered by controlling and changing the sintering pro-
cess parameters such as sintering temperature and pressure to
achieve the desired properties [183,293,294]. Therefore, it is
beneficial to investigate the role of GDL rigidity and
compressibility on the performance of URFCs in a range of
operating conditions and with different design parameters
(e.g. assembly pressure, gasket material and thickness, and the
flow field configuration). A factor that should be considered in
URFCs is that usually sintered titanium GDLs are used at oxy-
gen side and CGDLs are used at hydrogen side. Therefore, the
maximum assembly pressure can be limited to that can be
taken by the CGDL as it is more compressible and hence is more
affected by the clamping force.
Modifications of GDLs
Overview
Commonly, GDLs are treated and modified to improve the cell
performance mainly by addressing the water management
challenges. For CGDLs used in PEMFCs, the most common
treatments are PTFE-coating and implementation of MPL on
one or both sides of the GDL. Most of these treatments are
utilised to enhance the water transport in GDL to effectively
remove the product water and provide passage for effective
delivery of reactants to the active area. Omrani and Shabani
[48] have provided a detailed review on GDL modifications that
can be potentially applicable to GDLs for PEM-URFCs. Dis-
similar to the CGDLs in FCs, there are not many published
research studies available with a focus on improving the GDL
for URFCs. In this section, in addition to the URFC-focused
studies, relevant studies on PEM electrolysers are presented,
as the same GDLs are potentially applicable to URFCs.
Hydrophobisation
In PEMFCs, it is common to apply a hydrophobic agent such as
PTFE [57,60,61,99,100,295] or FEP [296e298] to improve water
management-related properties. It is shown that an optimal
amount of PTFE-coating can maximise the FC performance [299].
PTFE coating of GDL results in porosity reduction [300], hence
excessive amount of PTFE loading can hinder reactants trans-
port. However, in URFCs water management requirements are
paradoxical; in FC-mode, a more hydrophobic GDL is desired for
effective removal of the product water whereas in E-mode, a
hydrophilic GDL is more favourable to supply enough water to
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15
the catalyst area. Few articles have investigated the role of GDL
hydrophobicity in URFCs [57,60,61,95,99,100]. It is reported that
hydrogen-side GDL PTFE-coating does not affect the URFC per-
formance [61]. However, the FC performance of URFC is shown to
benefit from PTFE-coating of the oxygen-electrode GDL, while
there are contrary reports regarding the effect of GDL PTFE
coating on the electrolyser performance. The majority of re-
searchers have reported that in wet conditions, PTFE-coating of
GDL provides a significant improvement in FC-mode perfor-
mance [57,60,61,99,100]. Lower amounts of PTFE loading is
desirable as higher loading can block the GDL pore (lower diffu-
sivity) and hence hinder the oxygen transport. Ioroi et al. [61]
considered performance stability in their experimental study
and found that while PTFE loading of 8 mg cm3 provided the best
performance, however, the cyclic performance was not stable.
On the other hand, with PTFE loading of 16 mg cm3, perfor-
mance stability was achieved in addition to high roundtrip en-
ergy efficiency, though the performance was slightly lower
compared to using GDL with 8 mg cm3 PTFE loading. Several
research groups have reported that PTFE-coating of GDL has a
negative effect on the E-mode performance due to added resis-
tance for water (i.e. reactant) transport to the CL [61,95,301,302].
In contrast, Hwang et al. [57,60,99] reported that PTFE-coating
had no noticeable effect the E-mode performance; additionally,
they also reported that 10 wt% PTFE-coating of GDL in a PEM-
URFC with serpentine flow channel design, improved the E-
mode performance [100]. They argued that the PTFE-coated GDLs
resulted in lower cell resistance. This is contradictory with the
findings of other research papers. It is expected that PTFE-coating
increases the electrical resistance as PTFE is non-conductive.
Hwang et al. [57,60,99,100] investigated the effect of GDL
PTFE-coating on both FC and E-mode performance of PEM-
URFC. They found that PTFE loading can improve the FC per-
formance at dry (RH < 66%) [99] and fully wet (RH > 90%)
[57,60,99,100] conditions, while it deteriorates the performance
at moderate relative humidity of reactant gases [60,99]. How-
ever, in another study they reported that at dry conditions, the
PTFE loading has no significant effect on the FC performance
[57,303]. In another study [57], they investigated the effect of
the drying process on PTFE distribution in GDL and conse-
quently on the URFC performance. They reported that if the
drying stage was carried out is vacuum conditions, more uni-
form through-plane distribution of PTFE can be obtained in
Fig. 7 e Effect of Ti-GDL PTFE-coating on the stability of
URFC performance in FC-mode [95].
16 international journal of hydrogen energy xxx (xxxx) xxx
comparison with drying in atmospheric conditions. Their re-
sults indicated that higher PTFE concentration was obtained
close to the GDL surface when drying stage is performed in
atmospheric conditions that could reduce the FC performance
as liquid water can be trapped inside the GDL [57].
Wittstadt et al. [95] studied the effect of PTFE-coating on
the stability of the URFC performance in FC-mode. They found
that even at low current densities (<0.1 A cm1), the untreated
Ti-GDL can be flooded due to the accumulation of the water
product inside the hydrophilic pores of the bare Ti-GDL. This
effect can be seen in Fig. 7. After almost 60 min of URFC
operation in FC-mode, the performance was interrupted due
to the flooding using untreated GDL. However, PTFE coated
GDL exhibited a stable performance.
Zhuo et al. [304] investigated the effect of GDL PTFE-coating
on URFC performance by using carbon paper as GDL on both
sides. They examined three different loadings: 20.68 wt%,
26.95 wt%, and 29.97 wt%. The cell temperature was kept at
65  C; however, the values of reactants' inlet relative humidity
have not been reported. It is important to note that the relative
humidity of the reactants could have a significant effect on the
cell performance. They reported that a PTFE loading of 26.95 wt
% for the oxygen side GDL gave the optimal roundtrip efficiency.
In URFCs, some aspects of PTFE-coating have not been
investigated yet. To date, most of the research studies con-
ducted on the effect of GDL PTFE-coating on URFC perfor-
mance were carried out by having the cell temperature at high
temperatures such as 80  C [57,60,61,99,100]. However, there
are still some limited number of experimental studies that
were carried out at lower temperatures: such as that by
Wittstadt et al. [95] at 50  C and the study by Zhuo et al. [304]
conducted at 65  C that are not particularly low. The cell
temperature plays an important role in water management in
FC-mode [305e307]. As discussed before (Section Thermal
properties), higher temperatures mean more water evapora-
tion and hence more water removal from the cell in vapour
form. At lower temperatures in FC-mode, more liquid water is
present in the cell and there is higher chance of flooding,
especially by having hydrophilic or untreated GDLs [305e307].
PTFE-coating also affects both bulk and ICR of the GDL due to
partial insulation of the conductive material by PTFE [269,308].
In URFCs, this aspect of PTFE-coating has not been addressed
and this has remained as a gap in the literature to date. Hence,
it is recommended to investigate the effect of PTFE-coating of
the Ti-GDL on the cell resistance at different PTFE loadings.
Micro porous layer
In PEMFCs, the addition of MPL to GDL substrate is mainly to:
reduce mass transport limitations by enhancing water man-
agement, especially avoiding GDL flooding; reduce the inter-
facial electrical contact resistance between the CL and GDL;
provide support for CL and hence reduce the CL loss into GDL
[48,309]. Adding an MPL can avoid flooding but its exact role,
particularly on water transport, is yet to be fully understood.
The use of MPL has been reported to hinder flooding and
enhance the PEMFC performance [220,310e317] and also keep
the membrane hydrated in dry operating conditions [317]. In
PEMFCs, commonly MPL is formed by using a mixture of carbon
black (e.g. Vulcan® XC-72R [318] and Black Pearls® 2000 [319]) and
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hydrophobic agent (such as PTFE) applied on the GDL substrate.
The use of graphene to form MPL is suggested to improve the
PEMFC performance in both wet and dry operating conditions
compared to using MPLs based on carbon black [320,321]. Several
studies have highlighted the role of hydrophobic MPL in the
water management of PEMFCs in both normal [262,318,322,323]
and cold start [324] operations. A hydraulic barrier is formed by
the hydrophobic MPL and consequently, the water accumulated
in the catalyst layer needs to reach a higher pressure in order to
enter into the MPL pores [325]; as a result, the membrane is kept
hydrated at dry conditions [326]. In wet conditions, MPL en-
hances and stabilises the water removal from the cell, resulting
in performance improvement [310,318,327,328]. On the other
hand, it is reported that MPL can limit the diffusion of oxygen
into the CL [224] and reduce the GDL permeability by an order of
magnitude [329] in a dry GDL; therefore, a balanced design is
required to have the optimum performance. Also, it has been
suggested that the MPL density [330] and pore size distribution
[331] should be optimised depending on the operating conditions
(high or low relative humidity) to achieve the best performance.
Pore size distribution in MPL can be adjusted.
MPLs used in PEMFCs are mostly carbon-based [220,310e316].
However, as previously mentioned, carbon corrosion occurs
rapidly in E-mode. Compared to the PEMFCs, there have been a
very limited number of studies on MPL for URFCs [55, 59, 62, 91,
96e98, 131, 332]. The majority of these experiments use the
MPL mainly as a protective layer for the carbon-based GDL [55,
62, 96e98, 131, 332], which were discussed in section 2.1.2.
Hence the focus of previous studies was mainly on improving
the durability of CGDL rather than looking at its role similar to
the MPLs used in PEMFCs. Ito et al. [59,91] used titanium powder
loading to develop MPL on sintered Ti-felt (Fig. 8). The Ti particles
size used in their experiment was 20 mm, which was consider-
ably larger than the carbon powder size used in MPLs for PEMFCs
[220,310e316]. As a result, the pore sizes developed by this
method were larger (0.05e7 mm) compared to the MPLs used in
PEMFCs. The Ti-powder loading did not develop a uniform layer
similar to MPLs in PEMFCs as can be seen in Fig. 8b. Ti-powder
loadings were 110 mg cm3, 200 mg cm3, and 300 mg cm3.
No significant effect on the electrolyser performance was re-
ported by varying the Ti-powder loading. However, in FC-mode
operation, ti-powder loading was significantly effective in pre-
venting water flooding and improving the FC performance under
fully wet condition (inlet air with RH of 100%). On the other hand,
Ti-powder loading did not show much of improvement effect
under relatively dry conditions (inlet air RH of 66%) due to
different mass transport conditions of the water produced (ratio
between vapour and liquid phase) [59,91]. Contrary to the find-
ings of Ito et al. [59,91], Lettenmeier et al. [333] found that Ti-
powder loading can improve the electrolyser performance. For
PEM electrolyser, they have applied MPL (macro porous layer due
to larger pore size) by vacuum plasma spraying of Ti-powder on
sintered Ti-GDL for PEM electrolyser. The particles size used in
their experiment was <45 mm. The MPL reduced the ICR by
20 mU cm2 and mass transport limitations, especially at high
current densities. They have concluded that for water manage-
ment improvement at high current densities, next to the CL, low-
porosity Ti-layer is required and the layer close to the flow field
should have larger pore size for effective removal of product
oxygen.
 international journal of hydrogen energy xxx (xxxx) xxx
Fig. 8 e SEM images of (a) bare Ti-felt GDL and (b) Ti-felt GDL with Ti-powder loading. Ti-felt had a fibre [59].
In summary, it can be observed that MPL can have a posi-
tive effect on the performance of URFCs in fuel cell mode
similar to PEMFCs and possibly positive effect on E-mode as
well. Therefore, it is essential to further evaluate the effect of
using different materials, composition, and particle sizes, to
find an optimal MPL for URFCs.
Conclusions
Understanding the role of GDL in URFCs and the effect of
their properties on the overall performance can help improve
the performance, durability, and cost of URFCs that are
crucial for the commercialisation of this technology. A wide
range of studies have been conducted to improve the dura-
bility of GDL in URFCs, particularly in E-mode by applying
protective layers [55,62,96], structural modification of the
catalyst layer [56], and using titanium-based GDLs
[57,59,60,91e95]. The latter option has proven to be a viable
solution with satisfactory results in terms of durability;
however, it adds to the overall cost of URFC. Therefore,
investigation of other corrosion resistive alloys such as
stainless steel, Inconel, aluminium, and copper alloys with
proper coatings was suggested. The other two methods (i.e.
applying protective layers to GDL and structural modification
of the catalyst layer) have shown some potential; however,
long-term stability is still a concern and further investigation
is needed to prove their applicability.
The effect of GDL properties on roundtrip efficiency of
URFCs have been investigated in few articles and it has been
found that properties such as porosity and fibre diameter have
some impacts on the FC and E-modes performance. There are
some limited studies reported in the literature on the modi-
fications of GDLs such as PTFE-coating, titanium powder
loading, and Pt-coating to enhance the URFC performance,
especially in FC-mode; however, in general, in-depth charac-
terisation of GDLs properties such as permeability, diffusivity,
and electrical and thermal conductivities and their effects on
the URFC performance in FC and E-modes has remained to be
an obvious gap in the literature.
Considering the reported findings in the literature to date
for PEMFCs, and the modifications that are summarised by
Omrani and Shabani [48], several modifications can be
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
17
investigated for GDLs used in PEM-URFCs. These include:
perforation of the GDLs and creating water pathways to
improve the URFCs water management both in FC and E-
modes; design and evaluation of bimodal and gradient
porosity GDLs; identification of suitable materials and
composition to form MPL on a metal-based GDL suitable for
PEM electrolysis environment, and further investigation of the
GLD PTFE-coating impact on the roundtrip energy efficiency of
URFCs in different operating conditions.
Use of porous metals as GDL provides a great opportunity
to study the effect of the GDL properties on the FC and E-
modes performance. Manufacturing methods such as sin-
tering give more control over the properties such as porosity
and pore size. Therefore, compared to CGDLs it is more
practical to examine the effect of thickness, pore size, and
porosity while keeping the other factors constant. It has been
suggested that GDLs with gradient porosity can be beneficial
for effective water management and this type of GDLs can be
fabricated by sintering titanium powder, a method that is
already being used in biomedical [193] and precision filtering
[195] applications. Hence, it is recommended to investigate
the effect of GDL gradient porosity on the URFC performance.
Moreover, the research outcomes from the literature suggests
that the bimodal pore size distribution is favourable for water
management [138,153,213]; however, it has not been thor-
oughly investigated as CGDLs are not well-suited for this
purpose. Bimodal pore size distribution can be achieved by
powder metallurgy (by using spacers) to experimentally
investigate its effect on both FC and E-modes performance
and potentially improve the performance of URFCs.
In URFCs, switching from E-mode to FC-mode is a chal-
lenging task as the excess water must be removed from the
flow channels as well as the GDL while the membrane should
be kept hydrated. The properties of GDL such as porosity,
thickness, and water vapour diffusivity can affect the purging
requirements such as the required flow rate and duration
[112]. However, this aspect of GDL has not been investigated to
date. It is beneficial to examine the effect of different GDL
properties and possible treatments on purging characteristics
while switching between the modes.
Most of the research studies carried out on URFCs to date
are experimental and while there is a need for doing more
experimental research in this field, modelling at stack and
18 international journal of hydrogen energy xxx (xxxx) xxx
component levels needs to receive further attention. This is
crucial for better understanding of the role of different com-
ponents and operating conditions, the mechanisms of mass
transport, stack assembly, and their effects on the overall
performance of URFCs. Currently, there is no published
research concerning GDL modelling in URFCs and mathe-
matical modelling reported in the literature are mostly limited
to CGDLs in FCs. The results from studies on GDLs in PEMFCs
and limited studies on PEM electrolysers can be helpful in
terms of providing directions for preliminary development of
URFCs. However, dedicated studies are still required that
consider the dual role of GDLs in URFCs in both FC and E-
modes and the opposing requirements in these two modes.
Therefore, for improvement of design and performance along
with achieving cost reduction, it is critical to carry out dedi-
cated mathematical modelling in conjunction with experi-
mental studies.
Finally, it has been proven that applying MPL on GDLs used
in PEMFCs can significantly improve the cell performance in
certain operating conditions by improving the water man-
agement mainly. Hence it is worthwhile to investigate suitable
materials and compositions for MPL that can be applied to a
metal-based GDL and study the impact on the roundtrip effi-
ciency (i.e. both FC and E-modes performance). MPL can serve
three vital roles in a PEMFC, including: contact resistance
reduction; providing effective water management; and hin-
dering the loss of catalyst layer. Hwang et al. [59] used tita-
nium powder for this purpose in their experiments; however,
the particle size was much larger than the size of the carbon
black commonly used in commercial GDLs. Moreover, tita-
nium can form an oxide layer that increases the contact
resistance and hence lowers the performance. Therefore, use
of other corrosion resistive materials that are suitable for
electrolysis environment, such as TiN, for MPL preparation for
metallic GDLs needs further investigation.
Acknowledgement
The authors gratefully acknowledge the support through the
provision of an Australian Government Research Training
Program Scholarship at the School of Engineering, RMIT Uni-
versity, Australia.
references
[1] IEA. World energy outlook 2014. International Energy
Agency; 2014.
[2] Shabani B, Omrani R, Andrews J. Energy security and
sustainability for road transport sector: the role of hydrogen
fuel cell technology. In: Shukla A, Sharma A, editors. Energy
security and sustainability. Boca Raton: Taylor & Francis;
2017. p. 149e204.
[3] Andrews J, Shabani B. Re-envisioning the role of hydrogen
in a sustainable energy economy. Int J Hydrogen Energy
2012;37(2):1184e203.
[4] IPCC. Special report on renewable energy sources and
climate change mitigation. United Kingdom and New York,
NY, USA: Cambridge University Press; 2011.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
[5] Andrews J, Shabani B. Where does hydrogen fit in a
sustainable energy economy? Procedia Eng
2012;49(0):15e25.
[6] Andrews J, Shabani B. The role of hydrogen in a global
sustainable energy strategy. Wiley Interdiscipl Rev Energy
Environ 2014;3(5):474e89.
[7] Assaf J, Shabani B. Transient simulation modelling and
energy performance of a standalone solar-hydrogen
combined heat and power system integrated with solar-
thermal collectors. Appl Energy 2016;178:66e77.
[8] Assaf J, Shabani B. Economic analysis and assessment of a
standalone solar-hydrogen combined heat and power
system integrated with solar-thermal collectors. Int J
Hydrogen Energy 2016;41(41):18389e404.
[9] Islam MR, Shabani B, Rosengarten G. Nanofluids to improve
the performance of pem fuel cell cooling systems: a
theoretical approach. Appl Energy 2016;178:660e71.
[10] Shabani B, Andrews J, Subic A, Paul B. Novel concept of
long-haul trucks powered by hydrogen fuel cells. 2013.
p. 823e34.
[11] Maniatopoulos P, Andrews J, Shabani B. Towards a
sustainable strategy for road transportation in Australia:
the potential contribution of hydrogen. Renew Sustain
Energy Rev 2015;52:24e34.
[12] Frischauf N. 5 - hydrogen-fueled spacecraft and other space
applications of hydrogen a2 - ball, michael. In: Basile A,
Vezirog
lu TN, editors. Compendium of hydrogen energy.
Oxford: Woodhead Publishing; 2016. p. 87e107.
[13] Nguyen HQ, Aris AM, Shabani B. Pem fuel cell heat recovery
for preheating inlet air in standalone solar-hydrogen
systems for telecommunication applications: an exergy
analysis. Int J Hydrogen Energy 2016;41(4):2987e3003.
[14] Aris A, Shabani B. Sustainable power supply solutions for
off-grid base stations. Energies 2015;8(10):10904e41.
[15] Shabani B, Andrews J. Standalone solar-hydrogen systems
powering fire contingency networks. Int J Hydrogen Energy
2015;40(15):5509e17.
[16] Paul B, Andrews J. Optimal coupling of pv arrays to pem
electrolysers in solarehydrogen systems for remote area
power supply. Int J Hydrogen Energy 2008;33(2):490e8.
[17] Shabani B. Solar-hydrogen combined heat and power
systems for remote area power supply. In: School of
aerospace, mechanical and manufacturing engineering.
Melbourne, Australia: RMIT University; 2010.
[18] Shabani B. Solar-hydrogen combined heat and power
systems for remote area power supply. In: School of
aerospace, mechanical and manufacturing engineering.
RMIT University; 2010. p. 372.
[19] Assaf J, Shabani B. Experimental study of a novel hybrid
solar-thermal/pv-hydrogen system: towards 100%
renewable heat and power supply to standalone
applications. Energy 2018;157:862e76.
[20] Assaf J, Shabani B. Multi-objective sizing optimisation of a
solar-thermal system integrated with a solar-hydrogen
combined heat and power system, using genetic algorithm.
Energy Convers Manag 2018;164:518e32.
[21] Ball M, Weeda M. The hydrogen economy e vision or
reality?1. Int J Hydrogen Energy 2015;40(25):7903e19.
[22] Shabani B, Andrews J. Hydrogen and fuel cells. In:
Sharma A, Kar SK, editors. Energy sustainability through
green energy. India: Springer; 2015. p. 453e91.
[23] Lund PD, Lindgren J, Mikkola J, Salpakari J. Review of energy
system flexibility measures to enable high levels of variable
renewable electricity. Renew Sustain Energy Rev
2015;45(0):785e807.
[24] B. Shabani, J. Andrews and B. Sukhvinder, Fuel-cell heat
recovery, electrical load management, and the economics of
solar-hydrogen systems. Energy Power Systems 30 (4), 2010.
 international journal of hydrogen energy xxx (xxxx) xxx
[25] Kharel S, Shabani B. Hydrogen as a long-term large-scale
energy storage solution to support renewables. Energies
2018;11(10):2825.
[26] Moore J, Shabani B. A critical study of stationary energy
storage policies in Australia in an international context: the
role of hydrogen and battery technologies. Energies
2016;9(9):674.
[27] Shabani B, Biju M. Theoretical modelling methods for
thermal management of batteries. Energies 2015;8(9):
10153.
[28] Barbir F. Chapter one - introduction. In: Barbir F, editor. Pem
fuel cells. 2nd ed. Boston: Academic Press; 2013. p. 1e16.
[29] Altmann S, Kaz T, Friedrich KA. Bifunctional electrodes for
unitised regenerative fuel cells. Electrochim Acta
2011;56(11):4287e93.
[30] Mittelsteadt C, Norman T, Rich M, Willey J. Chapter 11 - pem
electrolyzers and pem regenerative fuel cells industrial
view. In: Garche PTM, editor. Electrochemical energy
storage for renewable sources and grid balancing.
Amsterdam: Elsevier; 2015. p. 159e81.
[31] Yim S-D, Park G-G, Sohn Y-J, Lee W-Y, Yoon Y-G, Yang T-H,
et al. Optimization of ptir electrocatalyst for pem urfc. Int J
Hydrogen Energy 2005;30(12):1345e50.
[32] Yim S-D, Lee W-Y, Yoon Y-G, Sohn Y-J, Park G-G, Yang T-H,
et al. Optimization of bifunctional electrocatalyst for pem
unitized regenerative fuel cell. Electrochim Acta
2004;50(2e3):713e8.
[33] Doddathimmaiah A, Andrews J. Theory, modelling and
performance measurement of unitised regenerative fuel
cells. Int J Hydrogen Energy 2009;34(19):8157e70.
[34] Bhansali G, Singh BP, Kumar R. Strategic optimisation of
microgrid by evolving a unitised regenerative fuel cell
system operational criterion. Int J Sustain Energy
2016;35(8):722e33.
[35] Cha vez-Ramı́rez AU, Cruz JC, Espinosa-Lumbreras R,
Ledesma-Garcı́a J, Duro  n-Torres SM, Arriaga LG. Design and
set up of a hybrid power system (pv-wt-urfc) for a stand-
alone application in Mexico. Int J Hydrogen Energy
2013;38(28):12623e33.
[36] Maclay JD, Brouwer J, Scott Samuelsen G. Dynamic analyses
of regenerative fuel cell power for potential use in
renewable residential applications. Int J Hydrogen Energy
2006;31(8):994e1009.
[37] Raj AS, Ghosh PC. Standalone pv-diesel system vs. Pv-h2
system: an economic analysis. Energy 2012;42(1):270e80.
[38] Bhogilla SS, Ito H, Kato A, Nakano A. Research and
development of a laboratory scale totalized hydrogen
energy utilization system. Int J Hydrogen Energy
2016;41(2):1224e36.
[39] Mitlitsky F, Myers B, Weisberg AH, Molter TM, Smith WF.
Reversible (unitised) pem fuel cell devices. Fuel Cell Bull
1999;2(11):6e11.
[40] Suppes GJ. Plug-in hybrid with fuel cell battery charger. Int J
Hydrogen Energy 2005;30(2):113e21.
[41] Suppes GJ. Roles of plug-in hybrid electric vehicles in the
transition to the hydrogen economy. Int J Hydrogen Energy
2006;31(3):353e60.
[42] Langemann M, Fritz DL, Muller M, Stolten D. Validation and
characterization of suitable materials for bipolar plates in
pem water electrolysis. Int J Hydrogen Energy
2015;40(35):11385e91.
[43] Jung H-Y, Huang S-Y, Ganesan P, Popov BN. Performance of
gold-coated titanium bipolar plates in unitized regenerative
fuel cell operation. J Power Sources 2009;194(2):972e5.
[44] Jung H-Y, Huang S-Y, Popov BN. High-durability titanium
bipolar plate modified by electrochemical deposition of
platinum for unitized regenerative fuel cell (urfc). J Power
Sources 2010;195(7):1950e6.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
19
[45] Zhang M, Hu L, Lin G, Shao Z. Honeycomb-like
nanocomposite ti-ag-n films prepared by pulsed bias arc
ion plating on titanium as bipolar plates for unitized
regenerative fuel cells. J Power Sources 2012;198(0):
196e202.
[46] Zhang H, Hou M, Lin G, Han Z, Fu Y, Sun S, et al.
Performance of tieag-deposited titanium bipolar plates in
simulated unitized regenerative fuel cell (urfc)
environment. Int J Hydrogen Energy 2011;36(9):5695e701.
[47] Yang G, Yu S, Mo J, Kang Z, Dohrmann Y, List FA, et al.
Bipolar plate development with additive manufacturing and
protective coating for durable and high-efficiency hydrogen
production. J Power Sources 2018;396:590e8.
[48] Omrani R, Shabani B. Gas diffusion layer modifications and
treatments for improving the performance of proton
exchange membrane fuel cells and electrolysers: a review.
Int J Hydrogen Energy 2017;42(47):28515e36.
[49] Millet P, Ngameni R, Grigoriev SA, Fateev VN. Scientific and
engineering issues related to pem technology: water
electrolysers, fuel cells and unitized regenerative systems.
Int J Hydrogen Energy 2011;36(6):4156e63.
[50] Sadhasivam T, Dhanabalan K, Roh SH, Kim TH, Park KW,
Jung S, et al. A comprehensive review on unitized
regenerative fuel cells: crucial challenges and
developments. Int J Hydrogen Energy 2017;42(7):4415e33.
[51] Paul B, Andrews J. Pem unitised reversible/regenerative
hydrogen fuel cell systems: state of the art and technical
challenges. Renew Sustain Energy Rev 2017;79:585e99.
[52] Barbir F. Chapter four - main cell components, material
properties, and processes. In: Barbir F, editor. Pem fuel cells.
2nd ed. Boston: Academic Press; 2013. p. 73e117.
[53] Jayakumar A, Sethu S, Ramos M, Robertson J, Al-Jumaily A.
A technical review on gas diffusion, mechanism and
medium of pem fuel cell. Ionics 2014;21(1):1e18.
[54] Cindrella L, Kannan AM, Lin JF, Saminathan K, Ho Y,
Lin CW, et al. Gas diffusion layer for proton exchange
membrane fuel cellsda review. J Power Sources
2009;194(1):146e60.
[55] Huang S-Y, Ganesan P, Jung H-Y, Popov BN. Development of
supported bifunctional oxygen electrocatalysts and
corrosion-resistant gas diffusion layer for unitized
regenerative fuel cell applications. J Power Sources
2012;198(0):23e9.
[56] Lee WH, Kim H. Optimization of electrode structure to
suppress electrochemical carbon corrosion of gas diffusion
layer for unitized regenerative fuel cell. J Electrochem Soc
2014;161(6):F729e33.
[57] Hwang C, Ito H, Maeda T, Nakano A, Kato A, Yoshida T.
Effect of through-plane polytetrafluoroethylene distribution
in a gas diffusion layer on a polymer electrolyte unitized
reversible fuel cell. ECS Trans 2013;58(1):1059e68.
[58] Ito H, Maeda T, Nakano A, Hwang CM, Ishida M, Yokoi N,
et al. Influence of different gas diffusion layers on the water
management of polymer electrolyte unitized reversible fuel
cell. ECS Trans 2010;33(1):945e54.
[59] Hwang CM, Ishida M, Ito H, Maeda T, Nakano A, Kato A,
et al. Effect of titanium powder loading in gas diffusion
layer of a polymer electrolyte unitized reversible fuel cell. J
Power Sources 2012;202(0):108e13.
[60] Hwang CM, Ishida M, Ito H, Maeda T, Nakano A,
Hasegawa Y, et al. Influence of properties of gas diffusion
layers on the performance of polymer electrolyte-based
unitized reversible fuel cells. Int J Hydrogen Energy
2011;36(2):1740e53.
[61] Ioroi T, Oku T, Yasuda K, Kumagai N, Miyazaki Y. Influence
of ptfe coating on gas diffusion backing for unitized
regenerative polymer electrolyte fuel cells. J Power Sources
2003;124(2):385e9.
20 international journal of hydrogen energy xxx (xxxx) xxx
[62] Chen G, Zhang H, Zhong H, Ma H. Gas diffusion layer with
titanium carbide for a unitized regenerative fuel cell.
Electrochim Acta 2010;55(28):8801e7.
[63] El-Kharouf A, Rees NV, Steinberger-Wilckens R. Gas
diffusion layer materials and their effect on polymer
electrolyte fuel cell performance e ex situ and in situ
characterization. Fuel Cell 2014;14(5):735e41.
[64] Holmstro € m N, Ihonen J, Lundblad A, Lindbergh G. The
influence of the gas diffusion layer on water management
in polymer electrolyte fuel cells. Fuel Cell 2007;7(4):
306e13.
[65] Zhan Z, Xiao J, Li D, Pan M, Yuan R. Effects of porosity
distribution variation on the liquid water flux through gas
diffusion layers of pem fuel cells. J Power Sources
2006;160(2):1041e8.
[66] Yau TC, Cimenti M, Bi X, Stumper J. Effects of cathode gas
diffusion layer design on polymer electrolyte membrane
fuel cell water management and performance. J Power
Sources 2011;196(22):9437e44.
[67] Lin G, Nguyen TV. Effect of thickness and hydrophobic
polymer content of the gas diffusion layer on electrode
flooding level in a pemfc. J Electrochem Soc
2005;152(10):A1942e8.
[68] Baik KD, Hong BK, Han K, Kim MS. Effects of anisotropic
bending stiffness of gas diffusion layers on the performance
of polymer electrolyte membrane fuel cells with bipolar
plates employing different channel depths. Renew Energy
2014;69(0):356e64.
[69] Baik KD, Kim SI, Hong BK, Han K, Kim MS. Effects of gas
diffusion layer structure on the open circuit voltage and
hydrogen crossover of polymer electrolyte membrane fuel
cells. Int J Hydrogen Energy 2011;36(16):9916e25.
[70] Reshetenko TV, Bender G, Bethune K, Rocheleau R. Effects
of local variations of the gas diffusion layer properties on
pemfc performance using a segmented cell system.
Electrochim Acta 2012;80(0):368e76.
[71] Reshetenko TV, St-Pierre J, Rocheleau R. Effects of local gas
diffusion layer gas permeability variations on spatial proton
exchange membrane fuel cells performance. J Power
Sources 2013;241(0):597e607.
[72] Morgan JM, Datta R. Understanding the gas diffusion layer
in proton exchange membrane fuel cells. I. How its
structural characteristics affect diffusion and performance.
J Power Sources 2014;251:269e78.
[73] Akiki T, Accary G, Charon W, Kouta R. Influence of local
porosity, local permeability, and contact resistance
between the gas diffusion layer and the bipolar plate, on the
performances of a polymer electrolyte membrane fuel cell.
In: 2nd internation conference on Communications,
Computing and Control Applications (CCCA); 2012. p. 1e6.
Marseilles, France.
[74] Qin Y, Li X, Du Q, Yin Y, Jiao K. Effect of wettability on water
removal from the gas diffusion layer surface in a novel
proton exchange membrane fuel cell flow channel. Int J
Hydrogen Energy 2013;38(29):12879e85.
[75] Darling RM, Khateeb S. The influence of gas-diffusion
layer properties on elevated temperature operation of
polymer-electrolyte fuel cells. J Power Sources
2013;243(0):328e35.
[76] Seo JH, Baik KD, Kim DK, Kim S, Choi JW, Kim M, et al.
Effects of anisotropic bending stiffness of gas diffusion
layer on the mea degradation of polymer electrolyte
membrane fuel cells by wet/dry gas. Int J Hydrogen Energy
2013;38(36):16245e52.
[77] Shou D, Tang Y, Ye L, Fan J, Ding F. Effective permeability of
gas diffusion layer in proton exchange membrane fuel cells.
Int J Hydrogen Energy 2013;38(25):10519e26.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
[78] Hirakata S, Mochizuki T, Uchida M, Uchida H, Watanabe M.
Investigation of the effect of pore diameter of gas diffusion
layers on cold start behavior and cell performance of
polymer electrolyte membrane fuel cells. Electrochim Acta
2013;108(0):304e12.
[79] Shou D, Fan J, Ding F. Effective diffusivity of gas diffusion
layer in proton exchange membrane fuel cells. J Power
Sources 2013;225(0):179e86.
[80] Zamel N, Li X. Effective transport properties for polymer
electrolyte membrane fuel cells e with a focus on the gas
diffusion layer. Prog Energy Combust Sci 2013;39(1):111e46.
[81] Hellstern T, Gauthier E, Cheah MJ, Benziger JB. The role of
the gas diffusion layer on slug formation in gas flow
channels of fuel cells. Int J Hydrogen Energy
2013;38(35):15414e27.
[82] Lu Z, Daino MM, Rath C, Kandlikar SG. Water management
studies in pem fuel cells, part iii: dynamic breakthrough
and intermittent drainage characteristics from gdls with
and without mpls. Int J Hydrogen Energy
2010;35(9):4222e33.
[83] Alhazmi N, Ingham DB, Ismail MS, Hughes KJ, Ma L,
Pourkashanian M. Effect of the anisotropic thermal
conductivity of gdl on the performance of pem fuel cells. Int
J Hydrogen Energy 2013;38(1):603e11.
[84] Roshandel R, Farhanieh B, Saievar-Iranizad E. The effects of
porosity distribution variation on pem fuel cell
performance. Renew Energy 2005;30(10):1557e72.
[85] Lin JF, Wertz J, Ahmad R, Thommes M, Kannan AM. Effect of
carbon paper substrate of the gas diffusion layer on the
performance of proton exchange membrane fuel cell.
Electrochim Acta 2010;55(8):2746e51.
[86] Maheshwari PH, Mathur RB, Dhami TL. The influence of the
pore size and its distribution in a carbon paper electrode on
the performance of a pem fuel cell. Electrochim Acta
2008;54(2):655e9.
[87] Banerjee R, Chevalier S, Liu H, Lee J, Yip R, Han K, et al. A
comparison of felt-type and paper-type gas diffusion layers
for polymer electrolyte membrane fuel cell applications
using x-ray techniques. J Electrochem Energy Convers
Storage 2018;15(1).
[88] Smolinka T, Ojong ET, Garche J. Chapter 8 - hydrogen
production from renewable energiesdelectrolyzer
technologies. In: Garche PTM, editor. Electrochemical
energy storage for renewable sources and grid balancing.
Amsterdam: Elsevier; 2015. p. 103e28.
[89] Yuan C-J, Wang C-L, Wu TY, Hwang K-C, Chao W-C.
Fabrication of a carbon fiber paper as the electrode and its
application toward developing a sensitive unmediated
amperometric biosensor. Biosens Bioelectron
2011;26(6):2858e63.
[90] Mathias MF, Roth J, Fleming J, Lehnert W. Diffusion media
materials and characterisation. In: Handbook of fuel cells.
John Wiley & Sons, Ltd; 2010.
[91] Ito H, Maeda T, Nakano A, Hwang CM, Ishida M, Kato A,
et al. Effect of titanium powder loading in microporous
layer on a polymer electrolyte unitized reversible fuel cell.
ECS Trans 2011;41(1):469e77.
[92] Sone Y. A 100-w class regenerative fuel cell system for lunar
and planetary missions. J Power Sources
2011;196(21):9076e80.
[93] Grigoriev SA, Millet P, Porembsky VI, Fateev VN.
Development and preliminary testing of a unitized
regenerative fuel cell based on pem technology. Int J
Hydrogen Energy 2011;36(6):4164e8.
[94] Grigoriev SA, Millet P, Dzhus KA, Middleton H, Saetre TO,
Fateev VN. Design and characterization of bi-functional
electrocatalytic layers for application in pem unitized
 international journal of hydrogen energy xxx (xxxx) xxx
regenerative fuel cells. Int J Hydrogen Energy
2010;35(10):5070e6.
[95] Wittstadt U, Wagner E, Jungmann T. Membrane electrode
assemblies for unitised regenerative polymer electrolyte
fuel cells. J Power Sources 2005;145(2):555e62.
[96] Song S, Zhang H, Ma X, Shao Z-G, Zhang Y, Yi B.
Bifunctional oxygen electrode with corrosion-resistive gas
diffusion layer for unitized regenerative fuel cell.
Electrochem Commun 2006;8(3):399e405.
[97] Alvar EN, Zhou B, Eichhorn SH. Oxidative treatment to
improve coating and electrochemical stability of carbon
fiber paper with niobium doped titanium dioxide sols for
potential applications in fuel cells. Electrochim Acta
2014;132:347e55.
[98] Jung H-Y, Ganesan P, Popov B. Development of high
durability bi-functional oxygen electrode for unitized
regenerative fuel cell (urfc). ECS Trans 2009;25(1):1261e9.
[99] Hwang C-M, Ishida M, Ito H, Maeda T, Nakano A, Kato A,
et al. Effect of ptfe contents in the gas diffusion layers of
polymer electrolyte-based unitized reversible fuel cells. J Int
Counc Electr Eng 2012;2(2):171e7.
[100] Hwang C, Ito H, Maeda T, Nakano A, Kato A, Yoshida T. Flow
field design for a polymer electrolyte unitized reversible fuel
cell. ECS Trans 2013;50(2):787e94.
[101] Millet P, Grigoriev SA, Porembskiy VI. Development and
characterisation of a pressurized pem bi-stack electrolyser.
Int J Energy Res 2013;37(5):449e56.
[102] Marangio F, Pagani M, Santarelli M, Calı̀ M. Concept of a
high pressure pem electrolyser prototype. Int J Hydrogen
Energy 2011;36(13):7807e15.
[103] Medina P, Santarelli M. Analysis of water transport in a high
pressure pem electrolyzer. Int J Hydrogen Energy
2010;35(11):5173e86.
[104] Millet P, Ngameni R, Grigoriev SA, Mbemba N, Brisset F,
Ranjbari A, et al. Pem water electrolyzers: from
electrocatalysis to stack development. Int J Hydrogen
Energy 2010;35(10):5043e52.
[105] Grigoriev SA, Millet P, Volobuev SA, Fateev VN.
Optimization of porous current collectors for pem water
electrolysers. Int J Hydrogen Energy 2009;34(11):4968e73.
[106] Kang Z, Mo J, Yang G, Retterer ST, Cullen DA, Toops TJ,
et al. Investigation of thin/well-tunable liquid/gas
diffusion layers exhibiting superior multifunctional
performance in low-temperature electrolytic water
splitting. Energy Environ Sci 2017;10(1):166e75.
[107] Mo J, Kang Z, Yang G, Retterer ST, Cullen DA, Toops TJ, et al.
Thin liquid/gas diffusion layers for high-efficiency
hydrogen production from water splitting. Appl Energy
2016;177:817e22.
[108] Steen III SM, Mo J, Kang Z, Yang G, Zhang FY. Investigation
of titanium liquid/gas diffusion layers in proton exchange
membrane electrolyzer cells. Int J Green Energy
2017;14(2):162e70.
[109] Feng K, Kwok DTK, Liu D, Li Z, Cai X, Chu PK. Nitrogen
plasma-implanted titanium as bipolar plates in polymer
electrolyte membrane fuel cells. J Power Sources
2010;195(19):6798e804.
[110] Hottinen T, Mikkola M, Mennola T, Lund P. Titanium sinter
as gas diffusion backing in pemfc. J Power Sources
2003;118(1e2):183e8.
[111] Rakousky C, Reimer U, Wippermann K, Carmo M, Lueke W,
Stolten D. An analysis of degradation phenomena in
polymer electrolyte membrane water electrolysis. J Power
Sources 2016;326:120e8.
[112] Ito H, Maeda T, Kato A, Yoshida T, Ulleberg Ø. Gas purge for
switching from electrolysis to fuel cell operation in polymer
electrolyte unitized reversible fuel cells. J Electrochem Soc
2010;157(7):B1072e80.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
21
[113] Zhang F-Y, Advani SG, Prasad AK. Performance of a metallic
gas diffusion layer for pem fuel cells. J Power Sources
2008;176(1):293e8.
[114] Feng-Yuan Z, Ajay KP, Suresh GA. Investigation of a copper
etching technique to fabricate metallic gas diffusion media.
J Micromech Microeng 2006;16(11):N23e7.
[115] Fushinobu K, Takahashi D, Okazaki K. Micromachined
metallic thin films for the gas diffusion layer of pefcs. J
Power Sources 2006;158(2):1240e5.
[116] Lee C-Y, Chuang C-W. A novel integration approach for
combining the components to minimize a micro-fuel cell. J
Power Sources 2007;172(1):115e20.
[117] Lee C-Y, Lin C-H. A novel integration approach for
combining the micro thermal sensor and stainless steel foil
as gas diffusion layer in micro fuel cell. Renew Energy
2010;35(4):759e62.
[118] Lee CY, Lee SJ, Lee YM, Chu KY. Integration of micro flow
sensor and flexible substrate as gdl in micro fuel cell. In: 4th
IEEE International Conference on Nano/Micro Engineered
and Molecular Systems; 2009. p. 637e40. Shenzhen, China.
[119] Blanco M, Wilkinson DP, Wang H, Liu SZS. Engineered gas
diffusion layers for proton exchange membrane fuel cells.
ECS Trans 2009;25(1):1507e18.
[120] Blanco M, Wilkinson DP, Wang H. Application of water
barrier layers in a proton exchange membrane fuel cell for
improved water management at low humidity conditions.
Int J Hydrogen Energy 2011;36(5):3635e48.
[121] Blanco M, Wilkinson DP, Wang H. Perforated metal sheets
as gas diffusion layers for proton exchange membrane fuel
cells. Electrochem Solid State Lett 2011;15(3):B20e3.
[122] Kumar A, Reddy RG. Materials and design development for
bipolar/end plates in fuel cells. J Power Sources
2004;129(1):62e7.
[123] Choi H, Kim O-H, Kim M, Choe H, Cho Y-H, Sung Y-E. Next-
generation polymer-electrolyte-membrane fuel cells using
titanium foam as gas diffusion layer. ACS Appl Mater
Interfaces 2014;6(10):7665e71.
[124] A.J. Cisar, O.J. Murphy, K.T. Jeng, C. Salinas, S. Simpson, D.
Weng, et al., Unitized barrier and flow control device for
electrochemical reactors. 2001, Google Patents.
[125] Hottinen T, Himanen O, Lund P. Effect of cathode structure
on planar free-breathing pemfc. J Power Sources
2004;138(1e2):205e10.
[126] Hamada A, Nakato K. Gas diffusion layer arrangement for a
fuel cell. US; 2002.
[127] Wilkinson DP, Campbell SA, Stumper J. Fuel cell with fluid
distribution layer having integral sealing capability. Ballard
Power Systems Inc; 2002.
[128] Yi P, Peng L, Lai X, Li M, Ni J. Investigation of sintered
stainless steel fiber felt as gas diffusion layer in proton
exchange membrane fuel cells. Int J Hydrogen Energy
2012;37(15):11334e44.
[129] Ma L, Sui S, Zhai Y. Investigations on high performance
proton exchange membrane water electrolyzer. Int J
Hydrogen Energy 2009;34(2):678e84.
[130] Roca-Ayats M, Garcı́a G, Galante JL, Pen ~ a MA, Martı́nez-
Huerta MV. Electrocatalytic stability of ti based-supported
pt3ir nanoparticles for unitized regenerative fuel cells. Int J
Hydrogen Energy 2014;39(10):5477e84.
[131] Sadhasivam T, Roh S-H, Kim T-H, Park K-W, Jung H-Y.
Graphitized carbon as an efficient mesoporous layer for
unitized regenerative fuel cells. Int J Hydrogen Energy
2016;41(40):18226e30.
[132] Williams MV, Begg E, Bonville L, Kunz HR, Fenton JM.
Characterization of gas diffusion layers for pemfc. J
Electrochem Soc 2004;151(8):A1173e80.
[133] Gostick JT, Fowler MW, Ioannidis MA, Pritzker MD,
Volfkovich YM, Sakars A. Capillary pressure and
22 international journal of hydrogen energy xxx (xxxx) xxx
hydrophilic porosity in gas diffusion layers for polymer
electrolyte fuel cells. J Power Sources 2006;156(2):375e87.
[134] Gostick JT, Fowler MW, Pritzker MD, Ioannidis MA,
Behra LM. In-plane and through-plane gas permeability of
carbon fiber electrode backing layers. J Power Sources
2006;162(1):228e38.
[135] Kowal JJ, Turhan A, Heller K, Brenizer J, Mench MM.
Liquid water storage, distribution, and removal from
diffusion media in pefcs. J Electrochem Soc
2006;153(10):A1971e8.
[136] Gao Y. Prediction the differences of permeability between
carbon fiber paper and carbon fiber cloth in pem fuel cells.
In: ASME 2011 9th international conference on fuel cell
science, engineering and technology. Collocated with ASME
2011 5th international conference on energy sustainability,
FUELCELL 2011; 2011.
[137] Radhakrishnan V, Haridoss P. Differences in structure and
property of carbon paper and carbon cloth diffusion media
and their impact on proton exchange membrane fuel cell
flow field design. Mater Des 2011;32(2):861e8.
[138] Gauthier E, Duan Q, Hellstern T, Benziger J. Water flow in,
through, and around the gas diffusion layer. Fuel Cell
2012;12(5):835e47.
[139] Gauthier E, Hellstern T, Kevrekidis IG, Benziger J. Drop
detachment and motion on fuel cell electrode materials.
ACS Appl Mater Interfaces 2012;4(2):761e71.
[140] Wang Y, Gundevia M. Measurement of thermal conductivity
and heat pipe effect in hydrophilic and hydrophobic carbon
papers. Int J Heat Mass Tran 2013;60(0):134e42.
[141] Feser JP, Prasad AK, Advani SG. Experimental
characterization of in-plane permeability of gas diffusion
layers. J Power Sources 2006;162(2):1226e31.
[142] Ralph TR, Hards GA, Keating JE, Campbell SA, Wilkinson DP,
Davis M, et al. Low cost electrodes for proton exchange
membrane fuel cells: performance in single cells and
ballard stacks. J Electrochem Soc 1997;144(11):3845e57.
[143] Moreira J, Sebastian PJ, Ocampo AL, Castellanos RH, Cano U,
Salazar MD. Dependence of pem fuel cell performance on
the configuration of the gas diffusion electrodes. J N Mater
Electrochem Syst 2002;5(3):173e5.
[144] Sasikumar G, Ryu H. Comparison of electrode backing
materials for polymer electrolyte membrane fuel cells. J
Korean Electrochem Soc 2003;6(3):183e6.
[145] Frey T, Linardi M. Effects of membrane electrode assembly
preparation on the polymer electrolyte membrane fuel cell
performance. Electrochim Acta 2004;50(1):99e105.
[146] Ihonen J, Mikkola M, Lindbergh G. Flooding of gas diffusion
backing in pefcs: physical and electrochemical
characterization. J Electrochem Soc 2004;151(8):A1152e61.
[147] Wang Y, Wang C-Y, Chen KS. Elucidating differences
between carbon paper and carbon cloth in polymer
electrolyte fuel cells. Electrochim Acta
2007;52(12):3965e75.
[148] Liao Y-K, Ko T-H, Liu C-H. Performance of a polymer
electrolyte membrane fuel cell with fabricated carbon fiber
cloth electrode. Energy Fuels 2008;22(5):3351e4.
[149] Yoshizawa K, Ikezoe K, Tasaki Y, Kramer D, Lehmann EH,
Scherer GG. Analysis of gas diffusion layer and flow-field
design in a pemfc using neutron radiography. J Electrochem
Soc 2008;155(3):B223e7.
[150] Park S, Popov BN. Effect of a gdl based on carbon paper or
carbon cloth on pem fuel cell performance. Fuel
2011;90(1):436e40.
[151] P.G. Stampino, L. Omati and G. Dotelli, Electrical
performance of pem fuel cells with different gas diffusion
layers. J Fuel Cell Sci Technol 8 (4), 2011.
[152] Basuli U, Jose J, Lee RH, Yoo YH, Jeong K-U, Ahn J-H, et al.
Properties and degradation of the gasket component of a
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
proton exchange membrane fuel cellda review. J Nanosci
Nanotechnol 2012;12(10):7641e57.
[153] Sasabe T, Deevanhxay P, Tsushima S, Hirai S. Investigation
on the effect of microstructure of proton exchange
membrane fuel cell porous layers on liquid water behavior
by soft x-ray radiography. J Power Sources
2011;196(20):8197e206.
[154] El-kharouf A, Mason TJ, Brett DJL, Pollet BG. Ex-situ
characterisation of gas diffusion layers for proton exchange
membrane fuel cells. J Power Sources 2012;218:393e404.
[155] Han M, Xu JH, Chan SH, Jiang SP. Characterization of gas
diffusion layers for pemfc. Electrochim Acta
2008;53(16):5361e7.
[156] Büchi F, Boillat P. Polymer electrolyte fuel cells, mass
transport. In: Kreysa G, Ota K-i, Savinell R, editors.
Encyclopedia of applied electrochemistry. New York:
Springer; 2014. p. 1661e9.
[157] Williams MV, Kunz HR, Fenton JM. Influence of convection
through gas-diffusion layers on limiting current in pem fcs
using a serpentine flow field. J Electrochem Soc
2004;151(10):A1617e27.
[158] Lum KW, McGuirk JJ. Three-dimensional model of a
complete polymer electrolyte membrane fuel cell e model
formulation, validation and parametric studies. J Power
Sources 2005;143(1e2):103e24.
[159] Hossain M, Islam SZ, Pollard P. Investigation of species
transport in a gas diffusion layer of a polymer electrolyte
membrane fuel cell through two-phase modelling. Renew
Energy 2013;51(0):404e18.
[160] Burlatsky SF, Atrazhev VV, Gummalla M, Condit DA, Liu F.
The impact of thermal conductivity and diffusion rates on
water vapor transport through gas diffusion layers. J Power
Sources 2009;190(2):485e92.
[161] Owejan JP, Owejan JE, Gu W, Trabold TA, Tighe TW,
Mathias MF. Water transport mechanisms in pemfc gas
diffusion layers. J Electrochem Soc 2010;157(10):B1456e64.
[162] Lin H-H, Cheng C-H, Soong C-Y, Chen F, Yan W-M.
Optimization of key parameters in the proton exchange
membrane fuel cell. J Power Sources 2006;162(1):246e54.
[163] Inamuddin I, Cheema TA, Zaidi SMJ, Rahman SU. Three
dimensional numerical investigations for the effects of gas
diffusion layer on pem fuel cell performance. Renew Energy
2011;36(2):529e35.
[164] Maslan NH, Gau MM, Masdar MS, Rosli MI. Simulation of
porosity and ptfe content in gas diffusion layer on proton
exchange membrane fuel cell performance. J Eng Sci
Technol 2016;11(1):85e95.
[165] Larbi B, Alimi W, Chouikh R, Guizani A. Effect of porosity
and pressure on the pem fuel cell performance. Int J
Hydrogen Energy 2013;38(20):8542e9.
[166] Sahraoui M, Kharrat C, Halouani K. Two-dimensional
modeling of electrochemical and transport phenomena in
the porous structures of a pemfc. Int J Hydrogen Energy
2009;34(7):3091e103.
[167] Mason TJ, Millichamp J, Shearing PR, Brett DJL. A study of
the effect of compression on the performance of polymer
electrolyte fuel cells using electrochemical impedance
spectroscopy and dimensional change analysis. Int J
Hydrogen Energy 2013;38(18):7414e22.
[168] Ye DHH, Gauthier E, Cheah MJ, Benziger J, Pan M. The effect
of gas diffusion layer compression on gas bypass and water
slug motion in parallel gas flow channels. AIChE J
2015;61(1):355e67.
[169] Toghyani S, Moradi Nafchi F, Afshari E, Hasanpour K,
Baniasadi E, Atyabi SA. Thermal and electrochemical
performance analysis of a proton exchange membrane fuel
cell under assembly pressure on gas diffusion layer. Int J
Hydrogen Energy 2018;43(9):4534e45.
 international journal of hydrogen energy xxx (xxxx) xxx
[170] El-kharouf A, Steinberger-Wilckens R. The effect of
clamping pressure on gas diffusion layer performance in
polymer electrolyte fuel cells. Fuel Cell 2015;15(6):802e12.
[171] Zhou W, Tang Y, Song R, Jiang L, Hui KS, Hui KN.
Characterization of electrical conductivity of porous metal
fiber sintered sheet using four-point probe method. Mater
Des 2012;37(0):161e5.
[172] Fang W-Z, Tang Y-Q, Chen L, Kang Q-J, Tao W-Q. Influences
of the perforation on effective transport properties of gas
diffusion layers. Int J Heat Mass Tran 2018;126:243e55.
[173] Nabovati A, Llewellin EW, Sousa ACM. A general model for
the permeability of fibrous porous media based on fluid
flow simulations using the lattice Boltzmann method.
Compos Appl Sci Manuf 2009;40(6e7):860e9.
[174] Van Doormaal MA, Pharoah JG. Determination of
permeability in fibrous porous media using the lattice
Boltzmann method with application to pem fuel cells. Int J
Numer Methods Fluid 2009;59(1):75e89.
[175] Cassie ABD, Baxter S. Wettability of porous surfaces. Trans
Faraday Soc 1944;40:546e51.
[176] Han B, Mo J, Kang Z, Zhang F-Y. Effects of membrane
electrode assembly properties on two-phase transport and
performance in proton exchange membrane electrolyzer
cells. Electrochim Acta 2016;188:317e26.
[177] Ito H, Maeda T, Nakano A, Hwang CM, Ishida M, Kato A,
et al. Experimental study on porous current collectors of
pem electrolyzers. Int J Hydrogen Energy
2012;37(9):7418e28.
[178] Ito H, Maeda T, Nakano A, Kato A, Yoshida T. Influence of
pore structural properties of current collectors on the
performance of proton exchange membrane electrolyzer.
Electrochim Acta 2013;100(0):242e8.
[179] Turkmen AC, Celik C. The effect of different gas diffusion
layer porosity on proton exchange membrane fuel cells.
Fuel 2018;222:465e74.
[180] Wan ZH, Zhong Q, Liu SF, Jin AP, Chen YN, Tan JT, et al.
Determination of oxygen transport resistance in gas
diffusion layer for polymer electrolyte fuel cells. Int J Energy
Res 2018;42(6):2225e33.
[181] Cuevas FG, Montes JM, Cintas J, Urban P. Electrical
conductivity and porosity relationship in metal foams. J
Porous Mater 2009;16(6):675e81.
[182] Jin MZ, Chen CQ, Lu TJ. The mechanical behavior of porous
metal fiber sintered sheets. J Mech Phys Solid
2013;61(1):161e74.
[183] Zhou W, Tang Y, Liu B, Song R, Jiang L, Hui KS, et al.
Compressive properties of porous metal fiber sintered sheet
produced by solid-state sintering process. Mater Des
2012;35(0):414e8.
[184] Nabovati A, Hinebaugh J, Bazylak A, Amon CH. Effect of
porosity heterogeneity on the permeability and tortuosity of
gas diffusion layers in polymer electrolyte membrane fuel
cells. J Power Sources 2014;248(0):83e90.
[185] Zhan Z, Xiao J, Zhang Y, Pan M, Yuan R. Gas diffusion
through differently structured gas diffusion layers of pem
fuel cells. Int J Hydrogen Energy 2007;32(17):4443e51.
[186] Karpenko-Jereb L, Sternig C, Fink C, Hacker V, Theiler A,
Tatschl R. Theoretical study of the influence of material
parameters on the performance of a polymer electrolyte
fuel cell. J Power Sources 2015;297:329e43.
[187] Huang Y-X, Cheng C-H, Wang X-D, Jang J-Y. Effects of porosity
gradient in gas diffusion layers on performance of proton
exchange membrane fuel cells. Energy 2010;35(12):4786e94.
[188] Xing L, Wang Y, Das PK, Scott K, Shi W. Homogenization of
current density of pem fuel cells by in-plane graded
distributions of platinum loading and gdl porosity. Chem
Eng Sci 2018;192:699e713.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
23
[189] Zhang Y, Verma A, Pitchumani R. Optimum design of
polymer electrolyte membrane fuel cell with graded
porosity gas diffusion layer. Int J Hydrogen Energy
2016;41(20):8412e26.
[190] Al-Smail JH. Optimal porosity design for gas diffusion layers
of hydrogen fuel cells. In: Proceedings of the conference on
summer computer simulation. Chicago, Illinois: Society for
Computer Simulation International; 2015. p. 1e6.
[191] Miyamoto Y, Kaysser WA, Rabin BH, Kawasaki A, Ford R.
Introduction. In: Miyamoto Y, et al., editors. Functionally
graded materials. Springer US; 1999. p. 1e6.
[192] Miyamoto Y, Kaysser WA, Rabin BH, Kawasaki A, Ford R.
Applications. In: Miyamoto Y, et al., editors. Functionally
graded materials. Springer US; 1999. p. 247e313.
[193] Wen CE, Yamada Y, Nouri A, Hodgson PD. Porous titanium
with porosity gradients for biomedical applications. Mater
Sci Forum 2007:720e5.
[194] Miao X, Sun D. Graded/gradient porous biomaterials.
Materials 2009;3(1):26e47.
[195] Tang HP, Wang J, Qian M. 28 - porous titanium structures and
applications. In: Qian M, Froes FH, editors. Titanium powder
metallurgy. Boston: Butterworth-Heinemann; 2015. p. 533e54.
[196] Qian M, Froes FH, editors. Titanium powder metallurgy.
Boston: Butterworth-Heinemann; 2015.
[197] He W, Yi JS, Van Nguyen T. Two-phase flow model of the
cathode of pem fuel cells using interdigitated flow fields.
AIChE J 2000;46(10):2053e64.
[198] Chun JH, Park KT, Jo DH, Kim SG, Kim SH. Numerical
modeling and experimental study of the influence of gdl
properties on performance in a pemfc. Int J Hydrogen
Energy 2011;36(2):1837e45.
[199] Lee J, Chevalier S, Banerjee R, Antonacci P, Ge N, Yip R, et al.
Investigating the effects of gas diffusion layer substrate
thickness on polymer electrolyte membrane fuel cell
performance via synchrotron x-ray radiography.
Electrochim Acta 2017;236:161e70.
[200] Mo J, Steen S, Han B, Kang Z, Terekhov A, Zhang F-Y, et al.
Investigation of titanium felt transport parameters for
energy storage and hydrogen/oxygen production. In: 13th
international energy conversion engineering conference.
American Institute of Aeronautics and Astronautics; 2015.
[201] Yao W, Yang J, Wang J, Nuli Y. Chemical deposition of
platinum nanoparticles on iridium oxide for oxygen
electrode of unitized regenerative fuel cell. Electrochem
Commun 2007;9(5):1029e34.
[202] Nitta I, Himanen O, Mikkola M. Contact resistance between
gas diffusion layer and catalyst layer of pem fuel cell.
Electrochem Commun 2008;10(1):47e51.
[203] Zhou Y, Jiao K, Du Q, Yin Y, Li X. Gas diffusion layer
deformation and its effect on the transport characteristics
and performance of proton exchange membrane fuel cell.
Int J Hydrogen Energy 2013;38(29):12891e903.
[204] Mortazavi M, Tajiri K. In-plane microstructure of gas
diffusion layers with different properties for pefc. J Fuel Cell
Sci Technol 2013;11(2). 021002-021002.
[205] Mortazavi M, Tajiri K. Liquid water breakthrough pressure
through gas diffusion layer of proton exchange membrane
fuel cell. Int J Hydrogen Energy 2014;39(17):9409e19.
[206] Tamayol A, Bahrami M. Water permeation through gas
diffusion layers of proton exchange membrane fuel cells. J
Power Sources 2011;196(15):6356e61.
[207] Nishida K, Murakami T, Tsushima S, Hirai S. Measurement
of liquid water content in cathode gas diffusion electrode of
polymer electrolyte fuel cell. J Power Sources
2010;195(11):3365e73.
[208] Han B, Steen III SM, Mo J, Zhang F-Y. Electrochemical
performance modeling of a proton exchange membrane
24 international journal of hydrogen energy xxx (xxxx) xxx
electrolyzer cell for hydrogen energy. Int J Hydrogen Energy
2015;40(22):7006e16.
[209] Siracusano S, Di Blasi A, Baglio V, Brunaccini G, Briguglio N,
Stassi A, et al. Optimization of components and assembling
in a pem electrolyzer stack. Int J Hydrogen Energy
2011;36(5):3333e9.
[210] Sun W, Peppley BA, Karan K. Modeling the influence of gdl
and flow-field plate parameters on the reaction distribution
in the pemfc cathode catalyst layer. J Power Sources
2005;144(1):42e53.
[211] Shahraeeni M, Hoorfar M. Pore-network modeling of liquid
water flow in gas diffusion layers of proton exchange
membrane fuel cells. Int J Hydrogen Energy
2014;39(20):10697e709.
[212] Santamaria AD, Das PK, MacDonald JC, Weber AZ. Liquid-
water interactions with gas-diffusion-layer surfaces. J
Electrochem Soc 2014;161(12):F1184e93.
[213] Cho J, Oh H, Park J, Min K, Lee E, Jyoung J-Y. Study on the
performance of a proton exchange membrane fuel cell
related to the structure design of a gas diffusion layer
substrate. Int J Hydrogen Energy 2014;39(1):495e504.
[214] Ko D, Doh S, Park HS, Kim MH. The analysis of adhesion
force at the interface of gas diffusion layer and channel in
polymer electrolyte membrane fuel cell. Int J Hydrogen
Energy 2018;43(33):16258e67.
[215] Ko D, Doh S, Park HS, Kim MH. The effect of through plane
pore gradient gdl on the water distribution of pemfc. Int J
Hydrogen Energy 2018;43(4):2369e80.
[216] Liu PS, Chen GF. Chapter two - making porous metals. In:
Chen PSLF, editor. Porous materials. Boston: Butterworth-
Heinemann; 2014. p. 21e112.
[217] Wang X-h, Li J-s, Hu R, Kou H-c, Zhou L. Mechanical
properties of porous titanium with different distributions of
pore size. Trans Nonferrous Metals Soc China
2013;23(8):2317e22.
[218] Hakamada M, Kuromura T, Chen Y, Kusuda H, Mabuchi M.
Influence of porosity and pore size on electrical resistivity
of porous aluminum produced by spacer method. Mater
Trans 2007;48(1):32e6.
[219] Januszewski J, Khokhar MI, Mujumdar AS. Thermal
conductivity of some porous metals. Lett Heat Mass Tran
1977;4(6):417e23.
[220] Qi Z, Kaufman A. Improvement of water management by a
microporous sublayer for pem fuel cells. J Power Sources
2002;109(1):38e46.
[221] Rashapov RR, Gostick JT. In-plane effective diffusivity in pemfc
gas diffusion layers. Transport Porous Media 2016:1e23.
[222] Rashapov R, Imami F, Gostick JT. A method for measuring
in-plane effective diffusivity in thin porous media. Int J Heat
Mass Tran 2015;85(0):367e74.
[223] Tranter TG, Stogornyuk P, Gostick JT, Burns AD, Gale WF. A
method for measuring relative in-plane diffusivity of thin
and partially saturated porous media: an application to fuel
cell gas diffusion layers. Int J Heat Mass Tran
2017;110:132e41.
[224] Chan C, Zamel N, Li X, Shen J. Experimental measurement
of effective diffusion coefficient of gas diffusion layer/
microporous layer in pem fuel cells. Electrochim Acta
2012;65(0):13e21.
[225] Zamel N, Astrath NGC, Li X, Shen J, Zhou J, Astrath FBG,
et al. Experimental measurements of effective diffusion
coefficient of oxygenenitrogen mixture in pem fuel cell
diffusion media. Chem Eng Sci 2010;65(2):931e7.
[226] Astrath NGC, Shen J, Song D, Rohling JH, Astrath FBG,
Zhou J, et al. The effect of relative humidity on binary gas
diffusion. J Phys Chem B 2009;113(24):8369e74.
[227] Yang L, Sun H, Fu X, Wang S, Jiang L, Sun G. A novel method
for effective diffusion coefficient measurement in gas
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
diffusion media of polymer electrolyte fuel cells. J Power
Sources 2014;257(0):80e3.
[228] Chevalier S, Lee J, Ge N, Yip R, Antonacci P, Tabuchi Y, et al.
In operando measurements of liquid water saturation
distributions and effective diffusivities of polymer
electrolyte membrane fuel cell gas diffusion layers.
Electrochim Acta 2016;210:792e803.
[229] Bruggeman DAG. Berechnung verschiedener physikalischer
konstanten von heterogenen substanzen. I.
Dielektrizita€ tskonstanten und leitfa€ higkeiten der
mischko € rper aus isotropen substanzen. Ann Phys
1935;416(7):636e64.
[230] Flückiger R, Freunberger SA, Kramer D, Wokaun A,
Scherer GG, Büchi FN. Anisotropic, effective diffusivity of
porous gas diffusion layer materials for pefc. Electrochim
Acta 2008;54(2):551e9.
[231] Zamel N, Li X, Shen J. Correlation for the effective gas
diffusion coefficient in carbon paper diffusion media.
Energy Fuels 2009;23(12):6070e8.
[232] Espinoza-Andaluz M, Andersson M, Sunde n B. Comparing
through-plane diffusibility correlations in pefc gas diffusion
layers using the lattice Boltzmann method. Int J Hydrogen
Energy 2017;42(16):11689e98.
[233] LaManna JM, Kandlikar SG. Determination of effective
water vapor diffusion coefficient in pemfc gas diffusion
layers. Int J Hydrogen Energy 2011;36(8):5021e9.
[234] Muirhead D, Banerjee R, George MG, Ge N, Shrestha P, Liu H,
et al. Liquid water saturation and oxygen transport
resistance in polymer electrolyte membrane fuel cell gas
diffusion layers. Electrochim Acta 2018;274:250e65.
[235] Neale GH, Nader WK. Prediction of transport processes
within porous media: diffusive flow processes within an
homogeneous swarm of spherical particles. AIChE J
1973;19(1):112e9.
[236] Tomadakis MM, Sotirchos SV. Ordinary and transition
regime diffusion in random fiber structures. AIChE J
1993;39(3):397e412.
[237] Nilsson L, Stenstro € m S. Gas diffusion through sheets of
fibrous porous media. Chem Eng Sci 1995;50(3):361e71.
[238] Mezedur MM, Kaviany M, Moore W. Effect of pore structure,
randomness and size on effective mass diffusivity. AIChE J
2002;48(1):15e24.
[239] Das PK, Li X, Liu Z-S. Effective transport coefficients in pem
fuel cell catalyst and gas diffusion layers: beyond
bruggeman approximation. Appl Energy 2010;87(9):2785e96.
[240] Dawes JE, Hanspal NS, Family OA, Turan A. Three-
dimensional cfd modelling of pem fuel cells: an
investigation into the effects of water flooding. Chem Eng
Sci 2009;64(12):2781e94.
[241] Wu R, Zhu X, Liao Q, Wang H, Ding Y-d, Li J, et al.
Determination of oxygen effective diffusivity in porous gas
diffusion layer using a three-dimensional pore network
model. Electrochim Acta 2010;55(24):7394e403.
[242] Hossain M, Islam SZ, Pollard P. Numerical study of the
effect of effective diffusivity and permeability of the gas
diffusion layer on fuel cell performance. Proc IME J Power
Energy 2012;226(7):907e21.
[243] Hwang GS, Weber AZ. Effective-diffusivity measurement of
partially-saturated fuel-cell gas-diffusion layers. J
Electrochem Soc 2012;159(11):F683e92.
[244] Nam JH, Kaviany M. Effective diffusivity and water-saturation
distribution in single- and two-layer pemfc diffusion
medium. Int J Heat Mass Tran 2003;46(24):4595e611.
[245] Moosavi SM, Niffeler M, Gostick J, Haussener S. Transport
characteristics of saturated gas diffusion layers treated with
hydrophobic coatings. Chem Eng Sci 2018;176:503e14.
[246] Orogbemi OM, Ingham DB, Ismail MS, Hughes KJ, Ma L,
Pourkashanian M. The effects of the composition of
 international journal of hydrogen energy xxx (xxxx) xxx
microporous layers on the permeability of gas diffusion
layers used in polymer electrolyte fuel cells. Int J Hydrogen
Energy 2016;41(46):21345e51.
[247] Tomadakis MM, Sotirchos SV. Transport properties of
random arrays of freely overlapping cylinders with
various orientation distributions. J Chem Phys
1993;98(1):616e26.
[248] He G, Yamazaki Y, Abudula A. A three-dimensional analysis
of the effect of anisotropic gas diffusion layer(gdl) thermal
conductivity on the heat transfer and two-phase behavior
in a proton exchange membrane fuel cell(pemfc). J Power
Sources 2010;195(6):1551e60.
[249] Sadeghifar H, Djilali N, Bahrami M. Thermal conductivity
of a graphite bipolar plate (bpp) and its thermal contact
resistance with fuel cell gas diffusion layers: effect of
compression, ptfe, micro porous layer (mpl), bpp out-of-
flatness and cyclic load. J Power Sources
2015;273:96e104.
[250] Alhazmi N, Ingham DB, Ismail MS, Hughes K, Ma L,
Pourkashanian M. The through-plane thermal conductivity
and the contact resistance of the components of the
membrane electrode assembly and gas diffusion layer in
proton exchange membrane fuel cells. J Power Sources
2014;270:59e67.
[251] Radhakrishnan A, Lu Z, Kandlikar SG. Effective thermal
conductivity of gas diffusion layers used in pemfc:
measured with guarded-hot-plate method and predicted by
a fractal model. Meet Abstr 2010;(10):932. MA2010e02.
[252] Thewsey DJ, Zhao YY. Thermal conductivity of porous
copper manufactured by the lost carbonate sintering
process. Phys Status Solidi 2008;205(5):1126e31.
[253] Karimi G, Li X, Teertstra P. Measurement of through-plane
effective thermal conductivity and contact resistance in
pem fuel cell diffusion media. Electrochim Acta
2010;55(5):1619e25.
[254] Sadeghi E, Djilali N, Bahrami M. Effective thermal
conductivity and thermal contact resistance of gas
diffusion layers in proton exchange membrane fuel cells.
Part 1: effect of compressive load. J Power Sources
2011;196(1):246e54.
[255] Sadeghifar H, Djilali N, Bahrami M. A new model for
thermal contact resistance between fuel cell gas diffusion
layers and bipolar plates. J Power Sources 2014;266(0):51e9.
[256] Sadeghifar H, Djilali N, Bahrami M. Effect of
polytetrafluoroethylene (ptfe) and micro porous layer (mpl) on
thermal conductivity of fuel cell gas diffusion layers: modeling
and experiments. J Power Sources 2014;248(0):632e41.
[257] Nitta I, Himanen O, Mikkola M. Thermal conductivity and
contact resistance of compressed gas diffusion layer of pem
fuel cell. Fuel Cell 2008;8(2):111e9.
[258] Burheim OS, Crymble GA, Bock R, Hussain N, Pasupathi S,
du Plessis A, et al. Thermal conductivity in the three layered
regions of micro porous layer coated porous transport
layers for the pem fuel cell. Int J Hydrogen Energy
2015;40(46):16775e85.
[259] Roy Chowdhury P, Vikram A, Phillips RK, Hoorfar M.
Measurement of effective bulk and contact resistance of gas
diffusion layer under inhomogeneous compression e part
ii: thermal conductivity. J Power Sources 2016;320:222e30.
[260] Chang T-C, Zhang J-P, Fuh Y-K. Electrical, mechanical and
morphological properties of compressed carbon felt
electrodes in vanadium redox flow battery. J Power Sources
2014;245:66e75.
[261] Smith DS, Alzina A, Bourret J, Nait-Ali B, Pennec F, Tessier-
Doyen N, et al. Thermal conductivity of porous materials. J
Mater Res 2013;28(17):2260e72.
[262] Thomas A, Maranzana G, Didierjean S, Dillet J, Lottin O.
Thermal and water transfer in pemfcs: investigating the
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
25
role of the microporous layer. Int J Hydrogen Energy
2014;39(6):2649e58.
[263] Zamel N, Becker J, Wiegmann A. Estimating the thermal
conductivity and diffusion coefficient of the microporous
layer of polymer electrolyte membrane fuel cells. J Power
Sources 2012;207(0):70e80.
[264] Aichlmayr HT, Kulacki FA. The effective thermal
conductivity of saturated porous media. In: George JPHAB-
C, Greene A, Young IC, editors. Advances in heat transfer.
Elsevier; 2006. p. 377e460.
[265] Woodside W, Messmer JH. Thermal conductivity of porous
media. Ii. Consolidated rocks. J Appl Phys 1961;32(9):1699e706.
[266] Zamel N, Li X, Shen J, Becker J, Wiegmann A. Estimating
effective thermal conductivity in carbon paper diffusion
media. Chem Eng Sci 2010;65(13):3994e4006.
[267] Hashin Z, Shtrikman S. A variational approach to the theory
of the effective magnetic permeability of multiphase
materials. J Appl Phys 1962;33(10):3125e31.
[268] Ashby MF. The properties of foams and lattices. Phil Trans
Math Phys Eng Sci 2006;364(1838):15e30.
[269] Sow PK, Prass S, Kalisvaart P, Me rida W. Deconvolution of
electrical contact and bulk resistance of gas diffusion layers
for fuel cell applications. Int J Hydrogen Energy
2015;40(6):2850e61.
[270] Selamet OF, Ergoktas MS. Effects of bolt torque and contact
resistance on the performance of the polymer electrolyte
membrane electrolyzers. J Power Sources
2015;281(0):103e13.
[271] Li G, Tan J, Gong J. Effect of compressive pressure on the
contact behavior between bipolar plate and gas diffusion
layer in a proton exchange membrane fuel cell. J Fuel Cell
Sci Technol 2014;11(4). 041009-041009.
[272] € Koç M. Contact resistance characteristics
Turan C, Cora ON,
of coated metallic bipolar plates for pem fuel cells e
investigations on the effect of manufacturing. Int J
Hydrogen Energy 2012;37(23):18187e204.
[273] Ismail MS, Damjanovic T, Ingham DB, Pourkashanian M,
Westwood A. Effect of polytetrafluoroethylene-treatment
and microporous layer-coating on the electrical
conductivity of gas diffusion layers used in proton
exchange membrane fuel cells. J Power Sources
2010;195(9):2700e8.
[274] Andre  J, Antoni L, Petit J-P, De Vito E, Montani A. Electrical
contact resistance between stainless steel bipolar plate and
carbon felt in pefc: a comprehensive study. Int J Hydrogen
Energy 2009;34(7):3125e33.
[275] Wu Z, Zhou Y, Lin G, Wang S, Hu SJ. An improved model for
predicting electrical contact resistance between bipolar
plate and gas diffusion layer in proton exchange membrane
fuel cells. J Power Sources 2008;182(1):265e9.
[276] Zhang L, Liu Y, Song H, Wang S, Zhou Y, Hu SJ. Estimation of
contact resistance in proton exchange membrane fuel cells.
J Power Sources 2006;162(2):1165e71.
[277] Mishra V, Yang F, Pitchumani R. Measurement and
prediction of electrical contact resistance between gas
diffusion layers and bipolar plate for applications to pem
fuel cells. J Fuel Cell Sci Technol 2004;1(1):2e9.
[278] Davies DP, Adcock PL, Turpin M, Rowen SJ. Bipolar plate
materials for solid polymer fuel cells. J Appl Electrochem
2000;30(1):101e5.
[279] Okel E, Schaar B, Kanoun O. Simultaneous measurement
of bulk and contact resistance of conductive materials for
fuel cells. In: Instrumentation and measurement
technology conference proceedings, 2008. IMTC 2008.
IEEE; 2008.
[280] Ye D, Gauthier E, Benziger JB, Pan M. Bulk and contact
resistances of gas diffusion layers in proton exchange
membrane fuel cells. J Power Sources 2014;256(0):449e56.
26 international journal of hydrogen energy xxx (xxxx) xxx
[281] Ismail MS, Ingham DB, Ma L, Pourkashanian M. The contact
resistance between gas diffusion layers and bipolar plates
as they are assembled in proton exchange membrane fuel
cells. Renew Energy 2013;52(0):40e5.
[282] Shian L, Jinliang Y, Martin A, Gongnan X, Bengt S. Influence
of anisotropic gas diffusion layers on transport phenomena
in a proton exchange membrane fuel cell. Int J Energy Res
2017;41(14):2034e50.
[283] Todd D, Schwager M, Me rida W. Three-dimensional
anisotropic electrical resistivity of pem fuel cell transport
layers as functions of compressive strain. J Electrochem Soc
2015;162(3):F265e72.
[284] Higier A, Liu H. Effects of the difference in electrical
resistance under the land and channel in a pem fuel cell. Int
J Hydrogen Energy 2011;36(2):1664e70.
[285] Carral C, Charvin N, Trouve  H, Me le
 P. An experimental
analysis of pemfc stack assembly using strain gage sensors.
Int J Hydrogen Energy 2014;39(9):4493e501.
[286] Zhang W, Wu C-w. Effect of clamping load on the
performance of proton exchange membrane fuel cell stack
and its optimization design: a review of modeling and
experimental research. J Fuel Cell Sci Technol 2013;11(2).
020801-020801.
[287] Li S, Sunden B. Effects of gas diffusion layer deformation on
the transport phenomena and performance of pem fuel
cells with interdigitated flow fields. Int J Hydrogen Energy
2018;43(33):16279e92.
[288] Qiu D, Janßen H, Peng L, Irmscher P, Lai X, Lehnert W.
Electrical resistance and microstructure of typical gas
diffusion layers for proton exchange membrane fuel cell
under compression. Appl Energy 2018;231:127e37.
[289] Ince UU, Marko € tter H, George MG, Liu H, Ge N, Lee J, et al.
Effects of compression on water distribution in gas
diffusion layer materials of pemfc in a point injection
device by means of synchrotron x-ray imaging. Int J
Hydrogen Energy 2018;43(1):391e406.
[290] Chen Y, Jiang C, Cho C. An investigation of the compressive
behavior of polymer electrode membrane fuel cell's gas
diffusion layers under different temperatures. Polymers
2018;10(9):971.
[291] Millichamp J, Mason TJ, Neville TP, Rajalakshmi N, Jervis R,
Shearing PR, et al. Mechanisms and effects of mechanical
compression and dimensional change in polymer
electrolyte fuel cells e a review. J Power Sources
2015;284(0):305e20.
[292] Bhosale AC, Mahajan MA, Ghosh PC. Optimization of
contact resistance with better gasketing for a unitized
regenerative fuel cell. Int J Hydrogen Energy 2018. in press,
https://doi.org/10.1016/j.ijhydene.2018.09.090.
[293] Zhou W, Tang Y, Pan M, Wei X, Xiang J. Experimental
investigation on uniaxial tensile properties of high-porosity
metal fiber sintered sheet. Mater Sci Eng
2009;525(1e2):133e7.
[294] Zhou W, Wang Q, Ling W, He L, Tang Y, Wu F, et al.
Characterization of three- and four-point bending
properties of porous metal fiber sintered sheet. Mater Des
2014;56(0):522e7.
[295] Chen Y, Tian T, Wan Z, Wu F, Tan J, Pan M. Influence of ptfe
on water transport in gas diffusion layer of polymer
electrolyte membrane fuel cell. Int J Electrochem Sci
2018;13(4):3827e42.
[296] Forner-Cuenca A, Biesdorf J, Lamibrac A, Manzi-Orezzoli V,
Büchi FN, Gubler L, et al. Advanced water management in
pefcs: diffusion layers with patterned wettability: ii.
Measurement of capillary pressure characteristic with
neutron and synchrotron imaging. J Electrochem Soc
2016;163(9):F1038e48.
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
[297] Lim C, Wang CY. Effects of hydrophobic polymer content in
gdl on power performance of a pem fuel cell. Electrochim
Acta 2004;49(24):4149e56.
[298] Yan W-M, Hsueh C-Y, Soong C-Y, Chen F, Cheng C-H, Mei S-
C. Effects of fabrication processes and material parameters
of gdl on cell performance of pem fuel cell. Int J Hydrogen
Energy 2007;32(17):4452e8.
[299] Chen T, Liu S, Zhang J, Tang M. Study on the characteristics
of gdl with different ptfe content and its effect on the
performance of pemfc. Int J Heat Mass Tran
2019;128:1168e74.
[300] Rashapov RR, Unno J, Gostick JT. Characterization of pemfc
gas diffusion layer porosity. J Electrochem Soc
2015;162(6):F603e12.
[301] Fall J, Humphreys D, Guo SM. Design and testing of a
unitized regenerative fuel cell. J Fuel Cell Sci Technol
2009;6(3). 031003-031003.
[302] Rabih S, Rallieres O, Turpin C, Astier S. Experimental study
of a pem reversible fuel cell. Renew Energy Power Qual J
2008;1(6):216e21.
[303] Ito H, Abe K, Ishida M, Hwang CM, Nakano A. Effect of
through-plane polytetrafluoroethylene distribution in a gas
diffusion layer on a polymer electrolyte unitized reversible
fuel cell. Int J Hydrogen Energy 2015;40(46):16556e65.
[304] Zhuo X, Sui S, Zhang J. Electrode structure optimization
combined with water feeding modes for bi-functional
unitized regenerative fuel cells. Int J Hydrogen Energy
2013;38(11):4792e7.
[305] Yin KM, Hsuen HK. Mathematical model of proton
exchange membrane fuel cell with consideration of water
management. Fuel Cell 2013;13(6):1213e25.
[306] Liu X, Guo H, Ye F, Ma CF. Flow dynamic characteristics in
flow field of proton exchange membrane fuel cells. Int J
Hydrogen Energy 2008;33(3):1040e51.
[307] Yan Q, Toghiani H, Causey H. Steady state and dynamic
performance of proton exchange membrane fuel cells
(pemfcs) under various operating conditions and load
changes. J Power Sources 2006;161(1):492e502.
[308] Rohendi D, Majlan EH, Mohamad AB, Daud WRW,
Kadhum AAH, Shyuan LK. Effect of ptfe content and
sintering temperature on the properties of a fuel cell
electrode backing layer. J Fuel Cell Sci Technol 2014;11(4).
041003-041003.
[309] Weber AZ, Newman J. Effects of microporous layers in
polymer electrolyte fuel cells. J Electrochem Soc
2005;152(4):A677e88.
[310] Deevanhxay P, Sasabe T, Tsushima S, Hirai S. Effect of
liquid water distribution in gas diffusion media with and
without microporous layer on pem fuel cell performance.
Electrochem Commun 2013;34(0):239e41.
[311] Ismail MS, Damjanovic T, Ingham DB, Ma L,
Pourkashanian M. Effect of polytetrafluoroethylene-
treatment and microporous layer-coating on the in-plane
permeability of gas diffusion layers used in proton
exchange membrane fuel cells. J Power Sources
2010;195(19):6619e28.
[312] Tseng C-J, Lo S-K. Effects of microstructure characteristics
of gas diffusion layer and microporous layer on the
performance of pemfc. Energy Convers Manag
2010;51(4):677e84.
[313] Kitahara T, Nakajima H, Mori K. Hydrophilic and
hydrophobic double microporous layer coated gas diffusion
layer for enhancing performance of polymer electrolyte fuel
cells under no-humidification at the cathode. J Power
Sources 2012;199:29e36.
[314] Kitahara T, Nakajima H, Inamoto M, Morishita M. Novel
hydrophilic and hydrophobic double microporous layer
 international journal of hydrogen energy xxx (xxxx) xxx
coated gas diffusion layer to enhance performance of
polymer electrolyte fuel cells under both low and high
humidity. J Power Sources 2013;234:129e38.
[315] Hiramitsu Y, Sato H, Hori M. Prevention of the water
flooding by micronizing the pore structure of gas diffusion
layer for polymer electrolyte fuel cell. J Power Sources
2010;195(17):5543e9.
[316] Kitahara T, Nakajima H, Inamoto M, Shinto K. Triple
microporous layer coated gas diffusion layer for
performance enhancement of polymer electrolyte fuel cells
under both low and high humidity conditions. J Power
Sources 2014;248:1256e63.
[317] Shan J, Lin R, Chen X, Diao X. Eis and local resolved current
density distribution analysis on effects of mpl on pemfc
performance at varied humidification. Int J Heat Mass Tran
2018;127:1076e83.
[318] €
Oztürk A, Fıçıcılar B, Erog _ Bayrakçeken Yurtcan A.

lu I,
Facilitation of water management in low pt loaded pem fuel
cell by creating hydrophobic microporous layer with ptfe,
fep and pdms polymers: effect of polymer and carbon
amounts. Int J Hydrogen Energy 2017;42(33):21226e49.
[319] Chen G, Zhang G, Guo L, Liu H. Systematic study on the
functions and mechanisms of micro porous layer on water
transport in proton exchange membrane fuel cells. Int J
Hydrogen Energy 2016;41(9):5063e73.
[320] Ozden A, Shahgaldi S, Li X, Hamdullahpur F. A graphene-
based microporous layer for proton exchange membrane
fuel cells: characterization and performance comparison.
Renew Energy 2018;126:485e94.
[321] Ozden A, Shahgaldi S, Zhao J, Li X, Hamdullahpur F.
Assessment of graphene as an alternative microporous
layer material for proton exchange membrane fuel cells.
Fuel 2018;215:726e34.
[322] Blanco M, Wilkinson DP. Investigation of the effect of
microporous layers on water management in a proton
exchange membrane fuel cell using novel diagnostic
methods. Int J Hydrogen Energy 2014;39(29):16390e404.
[323] Wu R, Zhu X, Liao Q, Wang H, Ding Y-d, Li J, et al. A pore
network study on the role of micro-porous layer in control
Please cite this article as: Omrani R, Shabani B, Review of gas diffusion layer for proton exchange membrane-based technologies with a
focus on unitised regenerative fuel cells, International Journal of Hydrogen Energy, https://doi.org/10.1016/j.ijhydene.2018.12.120
27
of liquid water distribution in gas diffusion layer. Int J
Hydrogen Energy 2010;35(14):7588e93.
[324] Xie X, Wang R, Jiao K, Zhang G, Zhou J, Du Q. Investigation
of the effect of micro-porous layer on pem fuel cell cold
start operation. Renew Energy 2018;117:125e34.
[325] Gostick JT, Ioannidis MA, Fowler MW, Pritzker MD. On the
role of the microporous layer in pemfc operation.
Electrochem Commun 2009;11(3):576e9.
[326] Weng F-B, Hsu C-Y, Su M-C. Experimental study of micro-
porous layers for pemfc with gradient hydrophobicity under
various humidity conditions. Int J Hydrogen Energy
2011;36(21):13708e14.
[327] Chen H-H, Chang M-H. Effect of cathode microporous layer
composition on proton exchange membrane fuel cell
performance under different air inlet relative humidity. J
Power Sources 2013;232:306e9.
[328] Zhou J, Shukla S, Putz A, Secanell M. Analysis of the role of
the microporous layer in improving polymer electrolyte fuel
cell performance. Electrochim Acta 2018;268:366e82.
[329] Orogbemi OM, Ingham DB, Ismail MS, Hughes KJ, Ma L,
Pourkashanian M. Through-plane gas permeability of gas
diffusion layers and microporous layer: effects of carbon
loading and sintering. J Energy Inst 2018;91(2):270e8.
[330] Cho J, Oh H, Park J, Min K, Lee E, Jyoung J-Y. Effect of the
micro porous layer design on the dynamic performance of a
proton exchange membrane fuel cell. Int J Hydrogen Energy
2014;39(1):459e68.
[331] Chun JH, Park KT, Jo DH, Lee JY, Kim SG, Lee ES, et al.
Determination of the pore size distribution of micro porous
layer in pemfc using pore forming agents under various
drying conditions. Int J Hydrogen Energy
2010;35(20):11148e53.
[332] Pai Y-H, Tseng C-W. Preparation and characterization of
bifunctional graphitized carbon-supported pt composite
electrode for unitized regenerative fuel cell. J Power Sources
2012;202(0):28e34.
[333] Lettenmeier P, Kolb S, Burggraf F, Gago AS, Friedrich KA.
Towards developing a backing layer for proton exchange
membrane electrolyzers. J Power Sources 2016;311:153e8.