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Frontiers of Materials Science

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ISSN 2095-0268(Online)

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Front. Mater. Sci.    2019, Vol. 13 Issue (3) : 217-241    https://doi.org/10.1007/s11706-019-0465-0
REVIEW ARTICLE
Graphene-based bipolar plates for polymer electrolyte membrane fuel cells
Ram Sevak SINGH1(), Anurag GAUTAM2, Varun RAI3
1. Department of Physics, O P Jindal University, Raigarh, Chhattisgarh 496109, India
2. Department of Chemistry, O P Jindal University, Raigarh, Chhattisgarh 496109, India
3. Department of Materials Science and Engineering, National University of Singapore, Singapore 117576, Singapore
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Abstract

Bipolar plates (BPs) are a major component of polymer electrolyte membrane fuel cells (PEMFCs). BPs play a multifunctional character within a PEMFC stack. It is one of the most costly and critical part of the fuel cell, and hence the development of efficient and cost-effective BPs is of much interest for the fabrication of next-generation PEMFCs in future. Owing to high electrical conductivity and chemical inertness, graphene is an ideal candidate to be utilized in BPs. This paper reviews recent advances in the area of graphene-based BPs for PEMFC applications. Various aspects including the momentous functions of BPs in the PEMFC, favorable features of graphene-based BPs, performance evaluation of various reported BPs with their advantages and disadvantages, challenges at commercial level products and future prospects of frontier research in this direction are extensively documented.
Keywords graphene      bipolar plate      polymer electrolyte membrane fuel cell      proton exchange membrane fuel cell     
Corresponding Author(s): Ram Sevak SINGH   
Online First Date: 23 September 2019    Issue Date: 29 September 2019
 Cite this article:   
Ram Sevak SINGH,Anurag GAUTAM,Varun RAI. Graphene-based bipolar plates for polymer electrolyte membrane fuel cells[J]. Front. Mater. Sci., 2019, 13(3): 217-241.
 URL:  
https://academic.hep.com.cn/foms/EN/10.1007/s11706-019-0465-0
https://academic.hep.com.cn/foms/EN/Y2019/V13/I3/217
Fig.1  Schematic showing the basic design of a PEMFC and its working principle.
Fig.2  (a)Icorr (corrosion current density) of several reported BPs. (b) ICR (interfacial contact resistance) of several reported BPs at 100–200 N·cm−2. The dot lines present the US-DOE 2020 targets of Icorr (<1 µA·cm−2) and ICR (<10 mΩ·cm2).
Fig.3  Power density of PEMFCs with several reported BPs. The dot line presents the US-DOE 2020 target of power density (>1 W·cm−2) of PEMFCs.
Material Disadvantages
Graphite Brittleness (poor mechanical strength), high weight and volume, and high processing cost
Metal Poor corrosion resistance or low surface conductivity (high ICR) due to the formation of protective surface oxide, and contamination of polymer membrane by dissolved metal ions (catalyst poisoning)
Carbon/carbon composites Low bulk electrical conductivity, low mechanical strength, and high cost
Polymer/metal composites Low electrical conductivity
Polymer/graphite composites Large volume and low corrosion resistance
Carbon/polymer composites Low electrical conductivity and mechanical strength
Stainless steel (SS) Inferior corrosion resistance or high ICR due to the formation of protective oxide films
a-C/SS Difficulty in mass production, corrosion resistance and ICR are generally does not meet the benchmark values (Icorr<1 µA·cm−2, ICR<10 mΩ·cm2)
Polymer/SS Inferior electrical conductivity
Gold/SS High cost
TiCx/a-C High cost, and challenges in mass production
TiN/Ti Highly expensive
TiN/SS High cost of processing
Fe/Ni/Cr Poor corrosion resistance and high ICR
SS/Zr2N2O High processing cost, and relatively low surface conductivity
Nb, Ti, Hf, Zr and Ta Too expensive for commercialization
Metal foams, carbon cloth Low corrosion resistance, high ICR, and complexity in mass production
Tab.1  Disadvantages of various bipolar plates
Fig.4  (a) Beneficial features of graphene-based BPs. Schematics showing graphene used (b) as coatings onto metallic BPs and (c) as conducting fillers in composite BPs.
Fig.5  (a) Corrosion rate of uncoated Cu and CVD grown graphene on Cu. (b) Corrosion rate of uncoated Ni and transferred two-layer graphene (tr2Gr/Ni) and four-layer graphene (tr4Gr/Ni) onto Ni. (Reproduced from Ref. [96] with permission of American Chemical Society)
Fig.6  STM images of CVD grown graphene on Pt(1 0 0) after corrosion tests in 0.513 mol·L−1 NaCl: (a)(b) corrosion tests at room temperature; (c) corrosion test at 60 °C. (Reproduced from Ref. [89] with permission of Royal Society of Chemistry)
Fig.7  (a) Photograph of graphene grown on Ni foam. (b) SEM image of graphene-coated Ni foam. (c) The schematic diagram of a single PEMFC consisting of graphene-coated Ni foam embedded within the groove of a graphite BP. (Reproduced from Ref. [126] with permission of Royal Society of Chemistry)
Fig.8  (a) Corrosion analysis (Tafel plot) of graphene-coated Ni foam (red curve) in an environment (H2SO4 (pH 1–1.5) + 2 ppm HF at 60 °C) simulating PEMFC operating conditions after 100 CV sweeps between −0.8 and+1.0 V (vs. OCP) at the scan rate of 25 mV·s−1. The black and blue curves represent Tafel plots of bare Ni foam and a-C/Ni foam, respectively. (b) SEM image of the graphene-coated Ni foam after corrosion test. The inset shows Raman spectra of graphene acquired from the graphene-coated Ni foam samples before and after corrosion tests. (Reproduced from Ref. [126] with permission of Royal Society of Chemistry)
Bipolar plate Corrosion environment Icorr
/(µA?cm−2)		 ICR
/(mΩ?cm2)		 P
/(mΩ?cm−2)		 Ref.
G/Ni-SS304 (CVD, multilayer G) 3.5% NaCl@RT 0.163 36 – [99]
G/SS304 3.5% NaCl@RT 35.2 – – [99]
SS304 3.5% NaCl@RT 7.41 560 – [99]
G/Cu (CVD, single layer G) PEMFC – – 415 [104]
Cu PEMFC – – 235 [104]
G/Cu (CVD, single layer G) 0.1 mol?L−1 NaCl@RT 0.28 – – [106]
Cu 0.1 mol?L−1 NaCl@RT 0.65 – – [106]
G/Al (transferred single layer G) 0.1 mol?L−1 NaCl@RT 2.8 – – [106]
G/Al (double layer G) 0.1 mol?L−1 NaCl@RT 3.0 – – [106]
G/Al (triple layer G) 0.1 mol?L−1 NaCl@RT 0.90 – – [106]
G/Al (quadruple layer G) 0.1 mol?L−1 NaCl@RT 1.80 – – [106]
Al 0.1 mol?L−1 NaCl@RT 0.23 – – [106]
rGO/SS316L 0.1 N H2SO4 + 2 ppm F−@80 °C 0.132 – 300 [107]
SS316L 0.1 N H2SO4 + 2 ppm F−@80 °C 0.14 120 [107]
Graphite 0.1 N H2SO4 + 2 ppm F−@80 °C – – 720.6 [107]
GO/Cu/MS (0.125 g·L−1 GO) 3.5% NaCl@RT 24.07 – – [110]
GO/Cu/MS (0.25 g·L−1 GO) 3.5% NaCl@RT 13.23 – – [110]
GO/Cu/MS (1 g·L−1 GO) 3.5% NaCl@RT 10.03 – – [110]
Cu/MS 3.5% NaCl@RT 68.60 – – [110]
Bare MS 3.5% NaCl@RT 316.5 – – [110]
rGO/Al (PVA-added coating) 0.5 mol?L−1 H2SO4@RT 0.003 – – [112]
rGO/Al (direct coating) 0.5 mol?L−1 H2SO4@RT 0.076 – – [112]
Bare Al 0.5 mol?L−1 H2SO4@RT 0.62 – – [112]
rGO/Al 2024 (spin coating) 3.5% NaCl@RT 0.254 – – [114]
Al 2024 3.5% NaCl@RT 719 – – [114]
rGO/Al (dip coating) 0.5 mol?L−1 NaCl@RT 0.0083 – – [115]
Al 0.5 mol?L−1 NaCl@RT 10.316 – – [115]
rGO/Sn/MS (electrodeposition) 3.5% NaCl@RT 0.815 – – [116]
Sn/MS 3.5% NaCl@RT 1.365 – – [116]
GO/Co/MS (electrodeposition) 3.5% NaCl@RT 3.04 – – [117]
Co/MS 3.5% NaCl@RT 9.70 – – [117]
rGO/Ni–P/MS 3.5% NaCl@RT 0.996 – [119]
Ni–P/MS 3.5% NaCl@RT 1.803 – [118]
G/Ni foam (CVD, multilayer G) H2SO4 (pH ~ 3) + 2 ppm HF@50 °C – – 640.8 [42]
TiN/Ni foam H2SO4 (pH ~ 3) + 2 ppm HF@50 °C – – 617.4 [42]
Au/Ni foam H2SO4 (pH ~ 3) + 2 ppm HF@50 °C – – 595.8 [42]
G/Ni foam (CVD, multilayer G) H2SO4 (pH ~ 3) + 2 ppm HF@80 °C 0.65 – – [42]
Ni foam H2SO4 (pH ~ 3) + 2 ppm HF@80 °C 3.5 – – [42]
TiN/Ni foam H2SO4 (pH ~ 3) + 2 ppm HF@80 °C 1.03 – – [42]
Au/Ni foam H2SO4 (pH ~ 3) + 2 ppm HF@80 °C 2.07 – – [42]
G/Ni foam (RTA, multilayer G) H2SO4 (pH ~ 1.5) + 2 ppm HF@70 °C 2.5 9.3 967 [126]
Ni foam H2SO4 (pH ~ 1.5) + 2 ppm HF@70 °C 98 – 521 [126]
a-C/Ni foam H2SO4 (pH ~ 1.5) + 2 ppm HF@70 °C 400 – 873 [126]
Tab.2  Summary of various reported graphene/metal BPs (crucial parameters such as corrosion current density (Icorr), interfacial contact resistance (ICR), and power density (P) of PEMFCs are comparatively presented)
Fig.9  (a) Water absorption of graphene-filled polybenzoxazine composites at various graphene loadings. Curves from top to down showing neat polybenzoxazine, 10, 20, 30, 40, 50 and 60 wt.% graphene loading, respectively. (b) Effect of the graphene contents on electrical conductivity of highly filled graphene/polybenzoxazine composites. (Reproduced from Ref. [128] with permission of Wiley)
Fig.10  (a) Tafel plots showing Icorr (corrosion current density) of optimum (1.5% rGO/30% NPFR/58.5% GP/5% CB/5% CF (1 mm in length)) composite BP at different conditions of PEMFC environment. (b) ICR of the composite BP vs. applied pressure. Here, rGO stands for reduced graphene, NPFR for novolac phenol formaldehyde resins, GP for graphite, CB for carbon black and CF for carbon fiber. (Reproduced from Ref. [133] with permission of Springer)
Bipolar plate Corrosion environment Icorr
/(µA?cm−2)		 σ
/(S?cm−1)		 ICR
/(mΩ?cm2)		 P
/(mW?cm−2)		 Ref.
G-NP/PPS (60 wt.% G-NP) a) – – 1.7 – – [127]
G-NP(l)/G-NP(s)/CB/PPS b) – – 114 – – [127]
G-NP/polybenzoxazine (10 wt.% G-NP) – – 1.52 – – [128]
G-NP/polybenzoxazine (20 wt.% G-NP) – – 2.50 – – [128]
G-NP/polybenzoxazine (30 wt.% G-NP) – – 7.42 – – [128]
G-NP/polybenzoxazine (40 wt.% G-NP) – – 9.26 – – [128]
G-NP/polybenzoxazine (50 wt.% G-NP) – – 125 – – [128]
G-NP/polybenzoxazine (60 wt.% G-NP) – – 357 – – [128]
G-NP/PP (7.5 wt.% G-NP) c) – – 5.28×10−11 – – [130]
Graphite/PP (7.5 wt.% graphite) – – 4.54×10−12 – – [130]
PP – – 1.21×10−16 – – [130]
rGO/PP-MAH/GP/CB/PP (2 wt.% rGO) d) – – 7.08±0.03 – – [131]
rGO/PP-MAH/GP/CB/PP (1 wt.% rGO) – – 9.78±0.15 – – [131]
rGO/PP-MAH/GP/CB/PP (0.5 wt.% rGO) – – 7.57±0.42 – – [131]
PP-MAH/GP/CB/PP – – 5.3±0.01 – – [131]
rGO/VER/GP/CB/CF (1 wt.% rGO) e) 1 mol?L−1 H2SO4 + 2 ppm HF@80 °C with O2 and H2 purging – 376.03 – 795 [132]
VER/GP/CB/CF 1 mol?L−1 H2SO4 + 2 ppm HF@80 °C with O2 and H2 purging – 355.05 – 723 [132]
rGO/NPFR/GP/CB/CF (1.5 wt.% rGO) f) 1 mol?L−1 H2SO4 + 2 ppm HF@80 °C with O2 and H2 purging 0.912 (anode), 0.988 (cathode) 319.42 14.73 342 [133]
NPFR/GP/CB/CF 1 mol?L−1 H2SO4+ 2 ppm HF@80 °C with O2 and H2 purging 0.734 (anode), 0.778 (cathode) 281.97 22.38 303 [133]
Tab.3  Summary of various reported graphene/polymer/metal BPs (crucial parameters such as corrosion current density (Icorr), electrical conductivity (σ), interfacial contact resistance (ICR), and power density (P) of PEMFC are comparatively presented)
Bipolar plate Corrosion environment Icorr/(µA·cm−2) c) Ref.
GO/PPY/SS304 (0.5 mg·mL−1 GO, electrodeposition) a) 0.1 mol·L−1 H2SO4@RT 0.40 [134]
GO/PPY/SS304 (1 mg·mL−1 GO) 0.1 mol·L−1 H2SO4@RT 0.059 [134]
GO/PPY/SS304 (1.5 mg·mL−1 GO) a) 0.1 mol·L−1 H2SO4@RT 0.120 [134]
PPY/SS304 a) 0.1 mol·L−1 H2SO4@RT 0.154 [134]
SS304 a) 0.1 mol·L−1 H2SO4@RT 7.70 [134]
rGO/PIHA/Cu (electrophoretic deposition) b) 3.5 wt.% NaCl@RT 4.0 [135]
Cu 3.5 wt.% NaCl@RT 38.25 [135]
Tab.4  Summary of various reported graphene/polymer/metal BPs
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