Exploring the potential of polyethylene/

epoxy/graphite composite as bipolar plate

material for proton exchange membrane fuel
cell
Cite as: AIP Conference Proceedings 2289, 020007 (2020); https://doi.org/10.1063/5.0028258
Published Online: 30 November 2020

O. A. Alo, I. O. Otunniyi and HCvZ Pienaar

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AIP Conference Proceedings 2289, 020007 (2020); https://doi.org/10.1063/5.0028258 2289, 020007

© 2020 Author(s).
 Exploring the Potential of Polyethylene/Epoxy/Graphite
Composite as Bipolar Plate Material for Proton Exchange
Membrane Fuel Cell

O. A. Alo1, 2, a), I. O. Otunniyi1, b), and HCvZ Pienaar 2, c)

1
Department of Metallurgical Engineering, Vaal University of Technology, Vanderbijlpark, South Africa
2
Centre for Alternative Energy, Vaal University of Technology, Vanderbijlpark, South Africa
a)
Corresponding author: 216074185@edu.vut.ac.za
b)
iyiolao@vut.ac.za
c)
christop@vut.ac.za

Abstract. On account of their low-cost, corrosion resistance, and lightweight, carbon-polymer composites (CPCs) are very
promising for producing bipolar plates (BPs) for proton exchange membrane fuel cells (PEMFCs). However, the substantial
conductive filler concentration that is required to give CPCs with the desired level of electrical conductivity for BP application
often results in difficulty in processing and degradation in mechanical strength. In this study, the potential of polyethylene
(PE)/epoxy/graphite composite to yield BPs with electrical and mechanical performance that meet the technical targets for
commercial PEMFC BPs was explored. PE/epoxy/graphite composites with varying graphite contents were prepared by melt
mixing followed by compression moulding. The morphology, flexural properties, and electrical conductivity of the composites
were investigated. The electrical conductivity and flexural modulus of the composites increased with increase in graphite
content while the flexural strength increased with graphite content up to a maximum of 42.1 MPa at 70 wt% graphite and then
decreased with further increase in graphite content. With respect to the United States Department of Energy (DOE) targets,
the PE/epoxy/80 wt% graphite composite has the most promising combination of electrical conductivity (72.96 Scm-1 for in-
plane and 4.12 Scm-1 for through-plane) and flexural strength (39.15MPa). Although the electrical conductivities of the
PE/epoxy/graphite composites are still below the DOE targets, achieving this level of conductivities with a single filler
indicates that the composites have promising potential for CPC BP applications.

INTRODUCTION

Bipolar plates (BPs) are critical components of the proton exchange membrane fuel cell (PEMFC) as their
functioning greatly impacts on the overall electrical and mechanical performance of the fuel cell stack. Carbon-
polymer composites (CPCs) have a huge potential for replacing the traditional graphite BP in PEMFCs. This is
due to their attractive properties such as good corrosion resistance, low cost, low density, and good formability.
A lot of research efforts have gone into developing CPC BPs that can meet the cost, performance, and durability
targets for PEMFC BPs.
For CPC BPs, the most difficult to achieve among the DOE technical requirements is the combination of the
required level of electrical performance and mechanical strength. This is because at high filler concentrations
necessary to impart adequate electrical conductivity, strength reduces with increase in filler contents due to weak
filler-matrix interface [1]. A possible solution to this problem is the use of polymers with inherent excellent
mechanical properties as matrices in CPC BPs. Polyethylene (PE) and epoxy resins have been extensively
investigated for application in CPC BPs. This is due to their attractive attributes. PE has low cost, good
processability, good toughness and impact resistance, and excellent chemical resistance. However, its
disadvantages are relatively low strength and stiffness [2]. Epoxy resins exhibit high mechanical strength, stiffness
and chemical resistance as well as high fluidity before curing, which allows for easy processing. However, they
are brittle and extremely prone to impact-induced failure due to their highly crosslinked structure [3]. Blending
of PE and epoxy resin has been reported to yield products with improved combination of strength, stiffness and
impact resistance [4]. Therefore, the combination of highly electrically conductive filler such as graphite with

Proceedings of PPS2019 Europe-Africa Regional Conference of the Polymer Processing Society

AIP Conf. Proc. 2289, 020007-1–020007-5; https://doi.org/10.1063/5.0028258
Published by AIP Publishing. 978-0-7354-4019-7/$30.00

020007-1
PE/epoxy blends has the potential to yield CPC BPs that will meet the performance and durability requirements
of commercial BPs.
In this study, PE/epoxy/graphite composites with varying graphite concentrations were produced by melt
mixing followed by compression molding. To assess their applicability in PEMFC BPs, the morphology, electrical
conductivity, and mechanical performance of the produced composites were investigated, and the results obtained
were compared to the DOE targets.

MATERIALS AND METHODS

Materials

The high density PE (Melt index 2.2 g/10 min) and polyethylene-grafted-maleic anhydride (PE-g-MAH) used
in this study were purchased from Sigma-Aldrich. The bisphenol-A epoxy resin (LR 30) and the amine-type
hardener (LH 30) were purchased from AMT Composites, South Africa. The densities of the epoxy resin and
harderner are 1.13 g/cm3 (at 25 oC) and 0.94 g/cm3 (at 20 oC) respectively. The graphite powder used was donated
by Graftech, South Africa.

Preparation of PE/Epoxy/Graphite Composites

Before mixing, the PE and PE-g-MAH were dried under vacuum at 70 oC for 8 hours to remove any moisture
that may be present. All composites were prepared by melt mixing in a Haake Rheomix OS mixer. The mixer was
preheated to 190 oC and mixing was carried out at 60 rpm rotor speed for a total processing time of 10 minutes.
Epoxy and PE are immiscible polymers. Therefore, the PE-g-MAH was used as compatibilizer to improve their
compatibility by ensuring a strong interfacial adhesion between the two polymers. An epoxy-PE weight ratio of
45:55 and epoxy-compatibilizer weight ratio of 3:1 were used. Also, an epoxy-hardener weight ratio of 5:1 was
used as recommended by the supplier. The graphite powder, PE and PE-g-MAH were first manually mixed. The
mixture was then transferred into the Rheomixer and mixed for 2 minutes. The epoxy resin was then added, and
mixing was continued for another 5 minutes. The hardener was then added, and the mixing was continued. After
a total mixing time of 10 minutes, the samples were taken out of the mixer and compression molded in a steel
mold of dimension 100 mm × 100 mm × 1.5 mm at 200 oC and 2 metric tonnes for 10 minutes. Different
PE/epoxy/graphite composite samples with graphite contents ranging from 30 to 80 wt. % were produced using
the above procedure. For comparison purpose, epoxy, PE/epoxy, epoxy/50 wt% graphite, and PE/50 wt% graphite
samples were also produced.

Characterization of Composite Samples

The morphology of the graphite filler, neat blend, and composites were examined using a scanning electron
microscope (TESCAN VEGA3). Prior to SEM observation, freeze-fractured samples of the blend and composites
were etched in dichloromethane for 30 min to remove the epoxy phase on the surfaces.
The flexural properties of the composite samples were measured at room temperature by the three-point
bending test using the Instron 5966 universal testing machining equiped with 10 KN load cell according to ASTM
D 790-03. The in-plane electrical conductivity measurements were carried out using the four-point probe method
according to ASTM D4496. During the through-plane conductivity measurements, each specimen was pressed
between two copper current collectors under a pressure of 140 Ncm-1 and the electrical resistance was measured
using a dual display LCR meter (Escort ELC-131D).

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 RESULTS AND DISCUSSION

Microstructure of the PE/Epoxy/Graphite Composites

The morphology of the graphite filler used in the study shows a layered structure (Fig. 1a). This type of
structure has the potentials for achieving higher conductivity CPCs compared to graphite particles with granular
structure [5]. However, the larger surface area can result into lower degree of filling and processability.
Fig. 1b shows the SEM micrographs of the fracture surfaces of the neat polymer blend. The PE/epoxy blend
exhibits a co-continuous morphology. The co-continuous morphology observed for the PE/epoxy blend can be
attributed to the close to symmetric composition of the blend. The morphology of the PE/epoxy/80 wt% graphite
composite is shown in Fig. 1c. At such high filler loading, the microstructure of the composite is largely influenced
by the morphology of the graphite filler. Therefore, the morphology of the PE/epoxy/80 wt% graphite composite
revealed flakes of graphite protruding from the polymer matrix. The graphite flakes are present throughout, and
no large, noticeable distinct polymeric features can be seen.

FIGURE 1. SEM micrograph of the (a) graphite filler (b); neat PE/epoxy blend; (c) PE/epoxy/80 wt% graphite composite

Flexural Properties of the PE/Epoxy/Graphite Composites

Fig. 2 shows the flexural strength for the neat epoxy, epoxy/50 wt% graphite, PE/50 wt% graphite, neat
PE/epoxy blend, and PE/epoxy/50 wt% graphite composite. Addition of 50 wt% graphite to the epoxy resin lowers
the flexural strength. Also, the flexural strength of the neat PE/epoxy (47.35 MPa) is lower than that of the neat
epoxy resin (67.11 MPa). Despite the considerable drop in flexural strength observed in the PE/epoxy blend
compared to the neat epoxy, the blend still retains enough flexural strength to make it a good candidate for matrix
in CPC BPs.
Comparing the epoxy resin, PE, and PE/epoxy, all filled with the same percentage of graphite, the strength
of the PE/epoxy/graphite composite is intermediate between that of the epoxy/graphite and PE/graphite. This can
be due to the inherent higher strength of epoxy compared to PE, coupled with the lower viscosity of the epoxy
resin at the elevated processing temperature, which would lead to better filler wetting and improve the matrix-
filler bonding strength. Fig. 3 shows the variation of the flexural properties of the PE/epoxy/graphite composites
with graphite content. The flexural modulus of the composites increased with increase in graphite content from
1661.43 MPa at 30 wt% graphite to 8860.61 MPa at 80 wt% graphite. This can be attributed to the inherent higher
stiffness of graphite compared to the polymer matrix, which would lead to lower strain and higher modulus as the
graphite content is increased. The flexural strength initially increased from 28.37 MP at 30 wt% to 42.10 MPa at
70 wt%. Further increase in amount of graphite to 80 wt% resulted in a decrease in flexural strength to 39.15 MPa.
The initial increase in flexural strength can be due to good matrix-filler adhesion, while the decrease in strength
at 80 wt% graphite can be attributed to poor matrix-filler adhesion as a result of insufficient amount of polymer
resin to completely wet the graphite filler within the composite.

Electrical Conductivity of the PE/Epoxy/Graphite Composites

The variation of in-plane electrical conductivity of the composite samples with graphite contents is shown in
Fig. 4a. The in-plane electrical conductivity of the composites increased as the graphite content increased from
30 to 80 wt%. The electrical conductivity of CPCs depends on mutual contact of the conductive filler materials to

020007-3
generate conductive paths throughout the composites. Therefore, increasing the graphite filler content would result
in more conductive paths for flow of current carrier within the composites, which is why the composite with the
highest graphite loading (80 wt%) exhibited the highest in-plane electrical conductivity.

80
70

Flexural strength (MPa) 60

50
40
30
20
10
0
Epoxy PE/graphite Epoxy/graphite PE/epoxy PE/epoxy/50
wt% graphite

FIGURE 2. Flexural strength of the neat epoxy resin and polymer blend, filled single polymers, and 50 wt. % graphite filled
polymer blend

Flexural strength Flexural modulus

50 10000
Flexural strength (MPa)

Flexural modulus (MPa)

40 8000

30 6000

20 4000

10 2000

0 0
20 30 40 50 60 70 80 90
Graphite content (wt%)

FIGURE 3. Flexural properties of the PE/epoxy/graphite composites

The conductivity values obtained in this study are below the target stipulated by the United States Department
of Energy (DOE), i.e., ˃100 Scm-1. However, the highest value obtained in this study (72.96 Scm-1, at 80 wt%
graphite) is higher than the values reported for several single polymer-matrix CPCs with similar filler loading in
previous studies [6]. The relatively high electrical conductivities obtained in this study can be attributed to the
immiscibility of the component polymers and the formation of a co-continuous morphology (Fig. 1b), which
would favor the distribution and concentration of the filler in one of the polymer phases and promote formation
of more continuous conducting paths. The through-plane electrical conductivities of the PE/epoxy/graphite
composites are shown in Fig. 4b. As in the case of in-plane conductivity, the through-plane electrical conductivity
increased from 0.20 Scm-1 at 30 wt% graphite to 4.12 Scm-1 at 80 wt% graphite. This can also be attributed to
formation of more conducting pathways within the composites as the graphite concentration increased.

020007-4
 4,5
[a] [b]

Through-plane conductivity (Scm-1)

80
4
In-plane conductivity (Scm-1)
70
60 3,5
3
50
2,5
40
2
30
1,5
20
1
10 0,5
0 0
20 30 40 50 60 70 80 90 20 30 40 50 60 70 80
Graphite content (wt%) Graphite content (wt%)
FIGURE 4. Electrical conductivity of the PE/epoxy composites: (a) in-plane; (b) through-plane

CONCLUSION

In this study, PE/epoxy/graphite composites with varying graphite contents were produced and characterized
in terms of morphology, electrical conductivity and flexural properties. The flexural strength of the composites
increased from 28.37 MPa at 30 wt% graphite to 42.10 MPa at 70 w% graphite, while further increase in graphite
content to 80 wt% resulted in decrease in the flexural strength to 39.15 MPa. The in-plane electrical conductivity
of the composites increased from 11.68 Scm-1 at 30 wt% graphite to 72.96 Scm-1 at 80 wt% graphite while the
through-plane conductivity increased from 0.20 Scm-1 at 30 wt% graphite to 4.12 Scm-1 at 80 wt%. Among the
produced composites, the PE/epoxy/80 wt% graphite composite is the most promising for PEMFC BP application
as it has the best combination of in-plane electrical conductivity and flexural strength with respect to the DOE
targets. The co-continuous morphology of the polymer matrix favours the concentration of the conductive filler
in one of the polymer phases, which would lead to formation of more conductive pathways and improved electrical
conductivity with increase in graphite content. The PE/epoxy/80 wt% graphite composite has the most promising
combination of electrical conductivity and flexural strength. Although, the electrical conductivity values obtained
in this study are below the DOE targets, the level of conductivities achieved indicates that PE/epoxy/graphite
composite has a promising potential for PEMFC BP applications.

ACKNOWLEDGMENTS

The National Research Foundation and Telkom Centre of Excellence of South Africa are appreciated for the
financial support for this work. Olawale Popoola and Uwa Orji (Tshwane University of Technology, South Africa)
are greatly appreciated for their support during the initial efforts on conductivity measurements.

REFERENCES

1. X. Jiang and L.T. Drzal, Journal of Power Sources 218, 297-306 (2012), doi:
10.1016/j.jpowsour.2012.07.001.
2. M. Kaseem, K. Hamad, F. Deri and Y.G. Ko, Polymer Science Series A 57(6) 689-703 (2015), doi:
10.1134/S0965545X15070068.
3. S. Chaudhary, S. Parthasarathy, V. Mangla, D. Kumar and P.K. Roy, Polymer-Plastics Technology and
Engineering 54(9) 907-915 (2015).
4. S. Pashaei, A.M.M. Siddaramaiah and A.A. Syed, ARPN Journal of Engineering and Applied Sciences
5(12) 26-37 (2010).
5. A. Király and F. Ronkay, Polymers and Polymer Composites 21(2) 93-100 (2013).
6. M.Y. Zakaria, A.B. Sulong, J. Sahari and H. Suherman, Composites Part B: Engineering 83 75-80 (2015).

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