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Understanding of the role of carbon fiber paper in PEMFCs

Article in Journal of Electrochemical Energy Conversion and Storage · February 2021

DOI: 10.1115/1.4050043

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Understanding of the Role of Carbon catalyst layer because catalyst particles easily drop into the macro-
pores during the preparation of GDL. Typically, commercially
Fiber Paper in Proton Exchange available GDL is generally dual structure (Fig. 2 [9]) consisting
of MPS possessing 1–300 µm uniform pores and MPL with a
Membrane Fuel Cells pore size no more than 1 µm [10].
In short, no matter what kind of GDL will involve MPS, or
Xiuyu Sun named BLs. MPS materials can be divided into two categories,
namely, carbon-based materials (carbon fiber paper, carbon fiber
School of Chemistry and Environmental Engineering, cloth, carbon felt, carbon black paper, etc.) and metal-based mate-
Shanghai Institute of Technology, rials. Carbon-based materials are widely adopted due to their
100# Haiquan Road, Fengxian District, good electrical conductivity, excellent acid resistance, better gas
Shanghai 201418, China permeability, unique resilience under assembly pressure, and poros-
e-mail: sunxiuyu1996@163.com ity retention ability. Carbon fiber paper and carbon cloth are often
used as GDL substrates for PEMFCs. The structural comparison

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Zhenwei Wang1
School of Chemistry and Environmental Engineering,
Shanghai Institute of Technology,
100# Haiquan Road, Fengxian District,
Shanghai 201418, China
e-mail: wangzhenwei@sit.edu.cn
Carbon fiber paper (CFP) is currently the main product of the
macroporous substrate (MPS) for the gas diffusion layer (GDL)
of proton exchange membrane fuel cells (PEMFCs). The optimiza-
tion of certain mechanical properties, electrical conductivity,
thermal conductivity, air conduction, and mass transfer capabilities
together with matched interaction can improve the core competi-
tiveness of CFP. The artical conducts a detailed theoretical analy-
sis of these conducting processes and principles based on CFP’s
main functions mentioned above. Thinner CFP with a wider pore
channel brings about better mass permeability but unsatisfactory
mechanical property. Thicker CFP with higher porosity and
rougher surface results in worse electrical and thermal conductiv-
ity. Meanwhile, the temperature, pressure, time, and other fabrica-
tion parameters of CFP are also discussed. With so many
contradictories, how to make a balance for real PEMFCs operation
and reduce the cost would be a practical strategy for the optimiza-
tion of CFP in the future. [DOI: 10.1115/1.4050043]
of carbon fiber paper and carbon cloth can be seen in Fig. 3 [11].
Combining the picture information with the specific data in
Table 1 shows that both of them have good electrical conductivity,
chemical stability, thermal stability, and corrosion resistance. Nev-
ertheless, carbon fiber paper has a lightweight, thinner thickness,
higher strength, smooth surface, lower contact resistance, more
uniform porosity, and especially better dimensional stability. The
preparation process of carbon paper is relatively simple and
mature with more stable performance. As a result, the carbon
fiber paper is the preferred material for the MPS of GDL.
2 Structure and Functions of Carbon Fiber Paper
2.1 Structure and Mechanical Properties. Figure 4 [12,13]
shows that CFP is a porous layer with a certain thickness composed
of randomly oriented carbon fibers [14]. Specifically, carbon fibers
and carbonized resins form a thin layer of stacked cylinders that
extend far more into the in-plane direction than the through-plane
direction [15]. The typical range of fiber diameter is between 3
and 10 µm, with CFP thickness in the range of 200–400 µm [16].
As shown in Fig. 1, the GDL made of CFP is placed vertically
between the catalytic layer and the bipolar plate during assembly.
It needs to support the catalytic layer and withstand the lateral
assembly pressure, while also resist gravity to keep it from

Keywords: carbon fiber paper, gas diffusion layer, proton

exchange membrane fuel cells, electrothermal property, mass
transfer management, fuel cells, thermal management

1 Introduction
Proton exchange membrane fuel cells (PEMFCs) is considered to
be one of the most promising alternative power supply for electric
vehicles, submarines, various movable power sources, power Fig. 1 Composition of PEMFC stack
grid, and fixed power supply due to their low operating temperature,
fast start-up speed, modular installation, and easy operation. GDL in
PEMFCs is located between the bipolar plate and the catalyst layers,
as shown in Fig. 1 [1]. It is a supporting structure of the catalyst
layer, a transmission channel for reaction gas, and water generated
from fuel cell as well as a vital structure for electronic and thermal
conduction [2–5]. GDL configured by either a single backing layer
(BL) composed of carbon-based materials, called macroporous sub-
strate (MPS), or a single-layer GDL with a thin microporous layer
(MPL) consisting of carbon black and polytetrafluoroethylene
(PTFE), or a dual-layer GDL with other substances [6–8]. The
macropores of single-layer GDL provides the effective transport
of gas and liquid water, while it also leads to poor support to the

1
Corresponding author.
Manuscript received September 25, 2020; final manuscript received January 29,
2021; published online February 23, 2021. Assoc. Editor: Partha P. Mukherjee. Fig. 2 Schematic diagram of a dual-layer GDL for PEMFC

Journal of Electrochemical Energy Conversion and Storage FEBRUARY 2022, Vol. 19 / 014501-1
Copyright © 2021 by ASME
 2.2 Electrical and Thermal Conductivity. Carbon fiber has a
graphite-like structure with graphite crystallites distributed inside,
making it difficult to slide between sheets. The graphite-like struc-
ture means that a large number of unlocalized π electrons exist
inside the carbon fiber (Fig. 5 [17]), and its large π bond unlocalized
area expands with the development of the graphite layer so that the
electrical conductivity of the fiber also increases.
The form of heat conduction of carbon fiber is lattice wave heat
transfer. Thermal conductivity is related to the free travel of the
phonon which can be represented by longitudinal acoustic (La) at
the graphite level. Larger La leads to greater thermal conductivity.
Electrical resistivity and thermal conductivity, as the two intrinsic
properties, are listed in Table 2 [18–22] and Table 3 [23–25]. The
electrical conductivity of graphite-like carbon materials is lower

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than that of most metals but far greater than that of nonmetals.
Graphite-structural substances possess almost the best thermal con-
ductivity, and the liquid water’s thermal conductivity is more than
20 times that of air as well as two times of specific resins. Further-
more, both the electrical and thermal conductivity of the parallel-
direction (longitudinal) outshine the perpendicular-direction
(radial).
There exist three elements that kick in the lateral electronic resis-
tance of GDL: raw material electronic conductivity, GDL thickness,
and gas channel width [26]. First, carbon fiber and resin residual
provide an electron pathway. According to Pouillet’s law

R = ρl/A (1)

where R is the electrical resistance, ρ is the electrical resistivity, l is

Fig. 3 Comparison of scanning electron microscope (SEM) for
(a) carbon paper (SGL 24BA) and (b) carbon cloth (E-Tek Cloth
“A”)
deforming. The analysis of the three-dimensional (3D) structure and
cross-sectional structure of carbon paper (Fig. 4) indicate that a
large number of carbon fiber layers are stacked after that the specific
resin connects them layer by layer, which ensures the shape stability
and good mechanical properties in both horizontal and vertical
directions. The bond strength between carbon fiber and specific
resin is the main factor affecting the performance of CFP.
the specimen length, and A is the cross-sectional area. Shorter
carbon fiber and larger fiber diameter contribute to decreased elec-
trical resistance. The electrical resistivity ρ decreases with the
increase of resin residual within a certain range [27]. When the
ideal value is exceeded, too much residual carbon causes the thick-
ness of the carbon paper to increase. Therefore, the carbon fibers are
relatively loose resulting in the contact resistance increases. Second,
thicker CFP has expanded cross-sectional area which is beneficial to
the increase of through-plane electrical resistance [28]. However,
too thinner CFP can cause permeation of catalyst into CFP, which
will cause ionic (and/or electronic conductivity) loss, and finally
voltage losses of the PEMFC [29,30]. Last, the growth of gas
channel width means the relative number of electronic channels
decreases, which leads to a loss on electrical conductivity. In addi-
tion, carbon fiber is a good conductor of electricity, its resistance
has a relatively small effect on battery performance [31–35]. So,
the contact resistance between the carbon paper and the bipolar
plate is the main source of contact resistance [36,37], which has a
greater impact on battery performance. The value of the contact
resistance is related to the material properties, surface morphology,

Table 1 Properties of carbon cloth and carbon paper

Product no. TGP-H-060 (Toray)a SGL 24BA (Sigracet) ELAT LT 1400W (Etek) Plain carbon cloth-1071 HCB (AvCarb)

Type Paper Paper Cloth Cloth

Thickness (mm) 0.19 0.19 0.454 0.356
Density (g/cm3) 0.44 0.80 – 1.50
Basic weight (g/cm2) – 54 170 132
Porosity (%) 78 84 63 –
Permeability 1900 ml · mm/(cm2 · hr · mmAq) 60 cm3/(cm2 · s)b 0.104 l/(m2 s Pa) –
Trough-plane resistance 80 mΩ cm <10 mΩ cm2c 0.17 mΩ cm2d –
Tensile strength 5 kgf/cm – – 19.25 Ncm
Flexural strength (MPa) 40 – – 345
Flexural modulus (GPa) 10 – – 51.7
PTFE treated Optional Yes Yes No
MPL No No Yes No
a
The standard size is a 400 mm square.
b
Gurley model 4118, 300 cc, 0.1 sq in orifice.
c
2-point measurement, circular (25 mm diam.) gold-plated contacts under pressure of 10 bars.
d
400 lb load using a 100 cm2 sample.

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Fig. 4 GDL, 3D reconstruction from µCT scans and SEM micrograph of cross section of CFP

Fig. 5 Microstructure of carbon fiber

Table 2 Electrical properties of different materials

Temperature coefficient,
Material Resistivity, ρ (Ω m) at 20 °C Conductivity, σ (S/m) at 20 °C (K−1) References

Copper 1.68 × 10−8 5.96 × 107 0.00404 [18]

Silicon 2.3 × 103 4.35 × 10−4 −0.075 [19]
Carbon (amorphous) 5 × 10−4 to 8 × 10−4 1.25 × 103 to 2.00 × 103 −0.0005 [20,21]
Carbon (graphite) parallel to basal plane 2.5 × 10−6 to 5.0 × 10−6 2 × 105 to 3 × 105 – [22]
Carbon (graphite) perpendicular to basal 3 × 10−3 3.3 × 102 – [22]
plane
PTFE 1023 to 1025 10−25 to 10−23 – –

and assembly pressure. The micro-morphology of the contact
surface makes the actual contact area much smaller than the
nominal contact area, resulting in repaid voltage loss on the
voltage–current curve. Increasing the assembly pressure can
increase the actual contact area and decrease the contact resistance,
while mass transfer may be hindered, and the battery may be
deformed, eventually causing the failure of a fuel cell.
As shown in the heat conduction equation
Q = ΔT/R = ΔTλS/L (2)
where Q is the total heat (unit, W), ΔT is the temperature difference
(unit, K), R is the thermal resistance (unit, K/W), λ is the thermal
conductivity (unit, W/(m K)), S is the area (unit, m2), and and L
is the thickness (unit, m).
Combined with the formula:
R = L/λS (3)
the equation:
λ = L/RS (4)
can be derived. For a specific material, the greater the thickness, the
worse the thermal conductivity. At the same time, combining the
data in Table 3, it can be seen that when the humidity increases,
the overall thermal conductivity of the system will increase. Simi-
larly, when the porosity increases, the thermal conductivity will
deteriorate. For controlling the temperature of the PEMFC stack,
the thermal conductivity from the contact surface also needs to be
paid attention to. Therefore, the surface of the CFP should be as
smooth as possible.
2.3 Transmission of Water and Reaction Gas. Proton
exchange membrane fuel cell is fed with hydrogen, which is oxi-
dized at the anode, and oxygen that is reduced at the cathode, at
the same time, water is produced as a reaction by-product (Fig. 6
[38]). The GDL located at the anode allows the hydrogen to
reach the reaction sites and wetting water vapor to maintain the
moisture of the PEM, while the cathode GDL transports oxygen
to the reaction point and discharges the reaction product water, as
shown in Fig. 7 [39]. The problem of cathode water management
is the most difficult and hot spot of research. When the battery
system is running, the mass transfer of gas and liquid occurs simul-
taneously, and there is a complex interaction between the two, so
the two are discussed together.
According to the modified equation of Fick’s law in diffusion
theory for porous medium:

Journal of Electrochemical Energy Conversion and Storage FEBRUARY 2022, Vol. 19 / 014501-3
 Table 3 Thermal properties of different materials

Materials Phase Thermal conductivity, λ (W/(m K)) Temperature (K) References

Graphene Solid (4840 ± 440) ∼ (5300 ± 480) 293 K [23]

Graphite Solid Longitudinal: 146–246 373–82 K [24]
radial: 92–175
Air Gas 0.026 300 K –
Water Liquid 0.596 293 K –
Phenolic Resin Solid ≈0.21 293 K [25]
PTFE Solid 0.25 298 K –

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Fig. 6 Schematic diagram of PEMFC

J = −(ε/τ)D∇C = −Deff ∇C (5)
where J is the diffusion flux, ɛ is the porosity, τ is the tortuosity, D is
the coefficient of diffusion, ∇C is the concentration gradient, Deff is
the effective diffusion coefficient, and “−” indicates that the diffu-
sion direction is the opposite direction of the concentration gradient,
that is, the diffusion from high concentration to low concentration.
However, the determination of tortuosity depends on the model
designed distinctly, so
Deff = D[ε(1 − S)] (n ≈ 1 − 3)
n
(6)
corrected by Bruggeman correlation and the empirical formula
Deff = Di ε1.5 (7)
Bernardi [40] has attracted most of the attention. The following
conclusion can be obtained: As the liquid water saturation (S)
increases and the porosity decreases, the Deff of the gas decreases
exponentially. The greater the porosity of the carbon paper, the
greater Deff and J, resulting in the better gas diffusion ability of
the carbon paper.
As shown in Fig. 3, the shapes of the pores in the medium, and
their level of connectedness are asymmetric. In-plane permeability
related to the porosity is used to describe the transport properties
more precisely. Permeability together with other relevant factors
that affect the mass transferability of carbon paper can be theoreti-
cally predicted by Darcy’s law (8) which describes the flow of a
fluid through a porous medium initially as well as Kozeny–
Carman equation (9)
ν = −(κΔp)/μL (8)
κ = ε3 /C(1 − ε)2 S2 (9)
ν is the gas/liquid velocity in units (m/s), κ is the permeability in
units (m2), Δp is the total pressure drop in units (Pa), μ is the
dynamic viscosity in units (Pa s), L us the length of the sample in
units (m); C is the KC constant, S is the specific surface area of
solid phase. Better porosity and smaller specific surface area of
medium are more favorable for permeability. Thinner CFP causes
a bigger concentration gradient, resulting in a larger amount of reac-
tants that can be transported into the catalyst layer. It’s mentioned
that more water generates following the increase of reactant gas,
which may consequently arouse the flooding problem to reduce
the PEMFC performance.
The management of cathode water is undoubtedly the research
hotspot. Regarding the dynamics of water transmission, a small
number of people think that it may be related to the temperature

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Fig. 7 Transportation route map of reaction gas, water, proton,
and electron at the cathode

gradient [41,42]. Most scholars believe that the capillary pressure Pc

is the main driving force for water transmission. Two different
views of specific transmission method of liquid water existed, one Fig. 9 Fingering schematic of the mechanism for liquid water
is a tree-like transmission [43,44] exhibited as Fig. 8 [43], the transport in GDL
other is a finger transmission [45–48] clarified by Fig. 9 [45]. More-
over, Manke et al. [49] pointed out that the two methods mentioned Table 4 Liquid water in various pores [50]
above both exist at the same time. Δp in Darcy’s law means the cap-
illary pressure (Pc) which is defined as the difference between gas Nature of pore Pc < 0 Pc = 0 Pc > 0
pressure (Pg) and liquid pressure (Pl). The critical pore size that
liquid water can enter is related to the capillary pressure and the Hydrophilic pore 0 ∼ rc,HI 0∼∞ 0∼∞
hydrophilic/hydrophobic surface properties of the pore wall: Hydrophobic pore 0a 0* rc,HO ∼ ∞
a
rc = 2σ cos θ/Pc (10) Indicates that liquid water cannot enter any pores.

where σ is the surface tension of liquid water, θ is the contact angle

of liquid water in the air on the surface of GDL. Table 4 [50] details
the infiltration state of liquid water to various pores in GDL. When
Pg > Pl, the gas can drive the liquid water to be discharged through
the hydrophilic pores (r < rc). When Pl predominates, the liquid
phase will occupy most of the pores, and the hydrophobic pores
provide channels for gas transportation to avoid flooding [51]. In
addition, researchers have verified that gradient porosity [52],
single statistical distribution porosity [53], and interval porosity
[54] lead to bimodal pore size distribution which contributes to
better mass transfer performance and battery performance.

Fig. 8 Rendering of water transport model, showing the branching

micro-to-macro-transport

Journal of Electrochemical Energy Conversion and Storage FEBRUARY 2022, Vol. 19 / 014501-5
 Fig. 10 Manufacture process of different carbon fiber paper
3 Preparation and Characterization of Carbon Fiber
Paper
Carbon fiber paper can be obtained by chopping carbon fibers
through a wet paper-making process. PAN-based, pitch-based
carbon fiber, and sometimes viscose-based carbon fiber are selected
as raw material. It can be divided into two parts which including
precursor molding and post-processing. Figure 10 details this repre-
sentative preparation process. First, the pre-treated chopped carbon
fiber is mixed with water, dispersants, and other additions uni-
formly, then the paper-making process is carried out, the carbon
fiber paper precursor (or carbon fiber felt) is obtained eventually.
After impregnation, molding, carbonization, and graphitization,
the carbon fiber paper is available.
High molecular weight polyethylene oxide (PEO), carboxy-
methyl cellulose (CMC), and anionic polyacrylamide (APAM)
are commonly used dispersants. Polyvinyl alcohol (PVA) has
high adhesion and excellent film-forming properties and is a com-
monly used adhesive. The purpose of impregnation is to introduce
adhesives to enhance the bonding force between carbon fibers. Phe-
nolic resin is easy to penetrate into the fiber, and after carbonization,
it has a high carbon content and a good carbonized structure. Gen-
erally, phenolic resin or modified phenolic is widely used in the
impregnation process and also acts as an adhesive. The molding
process solidifies the phenolic resin and obtains carbon fiber base
paper with certain flatness and strength. In the carbonization
process, part of the adhesive decomposes and shrinks in volume,
effectively reducing the density of the carbon fiber paper, increasing
the porosity, and reducing the resistivity. The graphitization process
further enhances the conductivity of CFP. In addition, since CFP is
used as the base material of the GDL, in order to better achieve the
gas–liquid mass transfer function, hydrophobic treatment is also
essential.
Abundantly properties and interaction of various materials, the
interaction between components of the battery and the adjustment
of process parameters during the preparation process or operating
conditions may all have a great impact on the quality and perfor-
mance of carbon fiber paper. Therefore, for the characterization
and analysis of carbon paper, it is not only necessary to statically
characterize the carbon paper itself, but also to test the performance
of the battery assembled with carbon paper and other components,
called dynamic characterization. The essential properties of carbon
fiber paper acting as backing layers are the thickness, density,
porosity, pore size distribution [55], permeability, specific resistiv-
ity, and contact resistance [56,57]. Moreover, surface morphology,
crystal structure, hydrophobic performance, and mechanical proper-
ties, such as tensile strength, also should be evaluated. Thickness
can be measured by Vernier caliper or computerized thickness
gauge, density can be measured by specific gravity balance, poros-
ity can be measured by porosity apparatus or by the weight differ-
ence between wet and dry carbon fiber paper, pore size distribution
can be measured by a capillary flowmeter and mercury intrusion
meter, permeability can be measured by air permeability apparatus,
specific resistivity can be measured by digital four-point probe
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measuring system [56], and contact resistance can be measured
by pressure measurement to designed device [57]. The scanning
electron microscope, universal testing machine, X-ray diffract-
ometer, etc., are also widely used in the characterization and analy-
sis of carbon fiber paper.
4 Summary and Prospect of Carbon Fiber Paper
As the base material of GDLs, carbon paper is placed vertically
between the bipolar plate and the catalyst layer as an important
role of PEMFCs. The optimization of electrical conductivity,
thermal conductivity, air conduction, and water transfer abilities
together with good interaction are the core competitiveness of
carbon paper, and certain mechanical properties provide the basis
for the realization of these abovementioned properties. However,
in most cases, the effects of a certain parameter change on the
above performance are contradictory. Electrical and thermal con-
ductivity as well as mechanical properties decrease as the porosity
of the carbon paper increases, but the mass transferability is the
opposite. A comprehensive evaluation of the physical, chemical,
and electrical properties of carbon paper requires the assembly of
single cells or battery packs under real conditions. This means
that there is no perfect carbon paper with fixed parameters, only
the fixed battery composition (determined proton exchange mem-
brane, catalyst, etc.) and the optimal carbon paper with the best rela-
tive performance under specific experimental conditions. Therefore,
long-term testing work is often required to determine the type of
carbon paper purchased.
Carbon paper has already completely marketed, available mainly
from Toray (Japan), SGL (German), Ballard and E-Tek (Canada),
and Carbon Energy Technology Company (Taiwan, China). A
large amount of research still focuses on the optimization of cost,
processes, materials, equipment, etc., far from industrial production
standards. Under the premise of ensuring the support performance,
gas–liquid mass transfer capability, and thermal and electric con-
ductivity, further reducing production costs, simplifying the
process flow, and increasing operability of carbon fiber paper will
contribute to the mass application of PEMFCs.
Conflict of Interest
There are no conflicts of interest.
Data Availability Statement
The datasets generated and supporting the findings of this article
are obtainable from the corresponding author upon reasonable
request. The authors attest that all data for this study are included
in the paper. No data, models, or code were generated or used for
this paper.
Transactions of the ASME
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FEBRUARY 2022, Vol. 19 / 014501-7