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Recent progress of Pt-based oxygen reduction reaction catalysts for proton exchange membrane fuel cells

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Abstract

With the increasing consumption of fossil fuels, proton exchange membrane fuel cells (PEMFCs) have attracted considerable attention as green and sustainable energy conversion devices. The slow kinetics of the cathodic oxygen reduction reaction (ORR) has a major impact on the performance of PEMFCs, and although platinum (Pt) can accelerate the reaction rate of the ORR, the scarcity and high cost of Pt resources still limit the development of PEMFCs. Therefore, the development of low-cost high-performance ORR catalysts is essential for the commercial application and development of PEMFCs. This paper reviews the research progress of researchers on Pt-based ORR catalysts in recent years, including Pt/C catalysts, Pt-based alloy catalysts, Pt-based intermetallic compounds, and Pt-based single-atom catalysts (SACs), with a focus on Pt-based alloy catalysts with different nanostructures. We described in detail the difficulties and solutions in the research process of various ORR catalysts and explained the principle of their activity enhancement with density functional theory (DFT). In addition, an outlook on the development of Pt-based catalysts is given, and reducing the amount of Pt used and improving the performance of catalysts are the directions to work on in the coming period.

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摘要

由于化石能源的加速消耗和日趋严重的环境问题, 质子交换膜燃料电池(PEMFCs)作为绿色可持续发展的能源转换装置引起了极大的关注。缓慢的阴极氧还原反应(ORR)动力学严重影响PEMFCs的性能, 虽然Pt可以加速ORR反应速率, 但是Pt资源的稀缺和昂贵的成本仍然限制了PEMFCs的发展。所以研究出低成本、高性能的ORR催化剂对于PEMFCs的商业化应用和发展至关重要。本文综述了近年来科研人员对于Pt基ORR催化剂的研究, 包括Pt/C催化剂、Pt基合金催化剂、Pt基金属间化合物、Pt基单原子催化剂, 其中重点讨论了不同纳米结构的Pt基合金催化剂。我们详细描述了各种ORR催化剂研究过程中的困难和解决办法, 并用密度泛函理论 (DFT) 解释了其活性提升的原理。此外, 还对Pt基催化剂的发展提出了展望, 开发低Pt、高效、稳定、经济和环保催化剂是今后一段时间需要努力的方向。

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Fig. 1

Reproduced with permission from Ref. [39]. Copyright 2022, American Chemical Society. d SEM images of graphene-Pt/C composites before and after cycling; e plot of ECSA versus number of turns obtained for catalysts cycled to 30,000 turns before and after Pickering emulsion treatment at between 0.60 and 0.95 V (vs. RHE). Reproduced with permission from Ref. [40]. Copyright 2022, John Wiley and Sons. f Pt-CNT@SnO2-T synthetic route schematic diagram; g valence band XPS spectrum of Pt-CNT@SnO2-T, where black dashed line indicates location of d-band center. Reproduced with permission from Ref. [59]. Copyright 2022, Elsevier

Fig. 2

Reproduced with permission from Ref. [104]. Copyright 2020, American Chemical Society. c HAADF-STEM image of Pt-Ni UHT; d schematic diagram of ORR catalytic layer of UHT for PEMFCs; e FFT results of Pt-Ni UHT. Reproduced with permission from Ref. [108]. Copyright 2022, American Chemical Society. DFT calculation results for f PtFe NW, g PtFe/Pt-V NW, and h PtFe/Pt NW for adsorption energy of oxygen-based intermediates; i activity volcano curve of PtFe/Pt NW. Reproduced with permission from Ref. [109]. Copyright 2021, Royal Society of Chemistry. J HAADF-STEM and EDS images of Pt-Co GB-NWs/C-OCP and Pt-Co SC-NWs; k dissolved amounts of Pt and Co during activation and durability test of Pt-Co GB-NWs/C-OCP and Pt-Co SC-NWs/C, where dissolved amounts have been normalized to total metal loading. Reproduced with permission from Ref. [110]. Copyright 2022, American Chemical Society

Fig. 3

Reproduced with permission from Ref. [113]. Copyright 2020, American Chemical Society. e Schematic diagram of synthesis of fct-Pt-Co@Pt octahedral nanocrystal catalyst with an ultra-thin Pt layer; f MA of catalysts at 0.9 V vs. RHE before and after different cycles of ADT. Reproduced with permission from Ref. [114]. Copyright 2021, American Chemical Society. g–j HAADF-STEM images and corresponding EDS elemental mapping of Pt-Ni PNCs; k, l line-scanning analysis along yellow and blue arrows in g, where arrows represent Ni scarcity; m MA and SA of Pt-Ni PNCs, Pt-Ni NWCs, and Pt-Ni PNs at 0.9 V vs. RHE (calculated from catalysts performing CV in Ar-saturated 0.1 mol·L−1 HClO4 and LSV in O2-saturated 0.1 mol·L−1 HClO4). Reproduced with permission from Ref. [118]. Copyright 2022, John Wiley and Sons. DFT-determined correlation of n overpotential and o atomic O binding energy relative to Pt (111) with coordination number of surface sites on each crystal plane during ORR. Reproduced with permission from Ref. [119]. Copyright 2022, American Chemical Society

Fig. 4

Reproduced with permission from Ref. [124]. Copyright 2022, Advanced Science. g Lattice spacing calculation for Pt-Cu-Mn UNFs (left) and Pt-Cu-Mn PNFs (right); h MA and SA at 0.9 V vs. RHE obtained by RDE testing of Pt-Cu-Mn UNFs, Pt-Cu-Mn PNFs and commercial samples in 0.1 mol·L−1 KOH solution. Reproduced with permission from Ref. [126]. Copyright 2020, john Wiley and Sons. i MA of PtCo-ND-NF at 0.9 V vs. RHE before and after ADT in 0.1 mol·L−1 HClO4 solution; j schematic diagram of synthesis of PtCo-ND-NF. Reproduced with permission from Ref. [125]. Copyright 2021, Elsevier

Fig. 5

Reproduced with permission from Ref. [140]. Copyright 2022, Elsevier. d Schematic diagram of kinetic energy barrier for transition from atomic disorder to atomic order; e cathodic MA of membrane electrode assemblies (MEAs) made with cathode catalysts of Pt/C and i-NP catalysts; f Fourier-transformed EXAFS data at Pt L3-edge of Pt3Co/S-C-600, Pt3Co/S-C-1000, and PtS2; g XPS spectra of Pt3Co/S-C-600 and S-C, indicating electronic interaction between metals and S-C, where a.u. is arbitrary units. Reproduced with permission from Ref. [143]. Copyright 2021, the American Association for the Advancement of Science. h PDOS of Pt and Pt1Co1-IMC@Pt. Reproduced with permission from Ref. [146]. Copyright 2022, Royal Society of Chemistry

Fig. 6

Reproduced with permission from Ref. [154]. Copyright 2021, John Wiley and Sons. d Schematic illustration for synthetic process of Pt1Con/N-GCNT encapsulated in a graphitic carbon nanotube; proposed ORR mechanism of e Pt1Co100/N-GCNT and f Pt2Co100/N-GCNT (gray, carbon; purple, cobalt; orange, platinum; red, oxygen; blue, hydrogen). Reproduced with permission from Ref. [155]. Copyright 2022, Elsevier. g Free energy diagram of different catalyst models; proposed ORR mechanisms based on h Pt3Co/in-plane Pt model and i Pt3Co/edged Pt model. Reproduced with permission from Ref. [157]. Copyright 2022, American Chemical Society

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Acknowledgements

This work was supported by CITIC Dameng Mining Industries Limited -Guangxi University Joint Research Institute of Manganese Resources Utilization and Advanced Materials Technology, Guangxi University-CITIC Dameng Mining Industries Limited Joint Base of Postgraduate Cultivation, and State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, and the National Natural Science Foundation of China (Nos.11364003 and 52102470), Guangxi Innovation Driven Development Project Grant (Nos. AA17204100 and AA18118052) and the Natural Science Foundation of Guangxi Province (No. 2018GXNSFAA138186).

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Authors and Affiliations

  1. School of Resources, Environment and Materials, Guangxi University, Nanning, 530004, China

    Feng Zhan, Kun-Song Hu, Jin-Hua Mai & Huan He

  2. School of Transportation Science and Engineering, Beihang University, Beijing, 102206, China

    Li-Sheng Zhang & Xin-Hua Liu

  3. IDTECH (Suzhou) Co. Ltd, Suzhou, 215217, China

    Zhen-Guo Zhang

  4. Dyson School of Design Engineering, Imperial College London, London, SW7 2AZ, UK

    Xin-Hua Liu

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Zhan, F., Hu, KS., Mai, JH. et al. Recent progress of Pt-based oxygen reduction reaction catalysts for proton exchange membrane fuel cells. Rare Met. 43, 2444–2468 (2024). https://doi.org/10.1007/s12598-023-02586-5

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