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Progress in Chemistry 2021, Vol. 33 Issue (3): 426-441 DOI: 10.7536/PC200612 Previous Articles   Next Articles

• Review •

Phosphoric Acid Based Proton Exchange Membranes for High Temperature Proton Exchange Membrane Fuel Cells

Yu Bai1, Shuanjin Wang1,*(), Min Xiao1,*(), Yuezhong Meng1, Chengxin Wang1   

  1. 1 Key Laboratory of Low-carbon Chemistry & Energy Conservation of Guangdong Province/State Key Laboratory of Optoelectronic Materials and Technologies, Sun Yat-sen University,Guangzhou 510275, China
  • Received: Revised: Online: Published:
  • Contact: Shuanjin Wang, Min Xiao
  • Supported by:
    the National Key Research and Development Program(Japan-China Joint Research Program)(2017YFE0197900); Link Project of the National Natural Science Foundation of China and Guangdong Province(U1601211); and the National Key Research and Development Program(2018YFA0702002)
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High temperature proton exchange membrane fuel cells(HT-PEMFCs) have many advantages over traditional proton exchange membrane fuel cells, which can not only enhance the catalysts tolerance to carbon monoxide poisoning, but also simplify the water and heat management as well as improve the energy conversion efficiency. Proton exchange membrane(PEM) is one of the key components of PEMFCs. Phosphoric acid(PA) doped PEMs have recently shown remarkable advantages due to the high proton conductivity and longevity at high operating temperatures(100~200 ℃) and low relative humidity. Generally, high PA doping level can improve the proton conductivity of PEMs, whereas the mechanical strength of the membranes dramatically deteriorates as an expense, therefore, enormous research on the synthesis of modified polymer electrolyte membranes with improved comprehensive performance has been carried out. This review focuses on the research progress of PA doped high temperature proton exchange membranes(HT-PEMs) such as polybenzimidazole and alkaline poly(aryl ether). Particularly, the application of porous materials including metal organic frameworks(MOFs) and covalent organic frameworks(COFs) in PEMs is also summarized. Finally, the remaining challenges in this filed are indicated.

Contents

1 Introduction

2 Proton conduction mechanism in proton exchange membranes

3 Challenges of HT?PEMs

4 Research progress on modification of phosphoric acid?based proton exchange membranes for HT?PEMFCs

4.1 Polybenzimidazole?based HT?PEMs

4.2 Non?polybenzimidazole?based HT?PEMs

5 Application of novel porous materials in HT?PEMFCs

5.1 Porous membranes based on PBI

5.2 MOFs

5.3 COFs

6 Conclusion and outlook

Key words: fuel cells, phosphoric acid doped, high temperature proton exchange membranes, polybenzimidazole, poly(aryl ether), MOFs, COFs
Fig.1 Repeat unit of m-PBI showing Lewis basic nitrogen atoms(green), “bonded acid”(blue), and “free acid”(red) at an acid doping level of 4 [16]
Fig.2 Conductivity mechanism of PA doped polybenzimidazoles:(a) water-acid proton transfer(b) proton transfer through a phosphoric acid chain and(c) benzimidazole ring-phosphoric acid proton transfer[4]
Fig.3 Synthesis of Ph-PBI and Me-PBI[40]
Fig.4 Synthesis of p-PPBI[42]
Fig.5 Chemical structures of SPBIs:(a) PBI-2Θ-1SO3H,(b) PBI-2Θ-2SO3H,(c) PBI-3Θ-1SO3H and(d) PBI-3Θ-3SO3H[44]
Fig.6 Synthesis of 2OHPBI[45]
Fig.7 Synthesis of OHPyPBI[46]
Fig.8 Interaction of P-MWCNTs with phosphoric acid doped PBI membranes, resulting in the formation of localized networks for efficient proton transport along the sidewalls of PMWCNTs[62]
Fig.9 Schematic of graphite oxide(GO) structure[63]
Fig.10 Presumed structures of self-reacted 2BIM-2Cl in crosslinked PBI(a) linear;(b) branched;(c) self-cross-linked[71]
Fig.11 Chemical structure of hyperbranched cross-linker Br-HPP[72]
Fig.12 Chemical structures of(a) branched F6PBI;(b) benzoxazine. The crosslinking sites are colored by blue and red, respectively
Fig.13 Schematic illustration of(a) ionically crosslinked blend membranes, and(b) the resulting covalently crosslinked blend membranes after heat cure[75]
Fig.14 Schematic illustration of cross-linked triazole modified poly(2,6-dimethyl-1,4-phenylene oxide) membranes(XTPPO)[14]
Fig.15 Proposed structural model of [Zn(H2PO4)2(C2N3H3)2]n(Zn∶P∶C∶N=1∶1.6∶4.1∶5.8), whereas the uncoordinated H3PO4 occupies the space where the monodentate H2P4- existed[118]
Fig.16 Chemical structure of Z-COF[132]
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