Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2024, Vol. 62: 156-165.DOI: 10.1016/S1872-2067(24)60067-7

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An efficient and stable high-entropy alloy electrocatalyst for hydrogen evolution reaction

Gui Zhaoa,b,c,1, Kuan Lud,1, Yunan Lie, Fagui Lua,b,c, Peng Gaoa,b,c, Bing Nane, Lina Lie, Yixiao Zhanga,b,c, Pengtao Xua,b,c,*(), Xi Liua,b,c,*(), Liwei Chena,b,c,*()   

  1. aSchool of Chemistry and Chemical Engineering, in-situ Center for Physical Sciences, Shanghai Jiao Tong University, Shanghai 200240, China
    bFrontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai 200240, China
    cShanghai Electrochemical Energy Device Research Center (SEED), Shanghai Jiao Tong University, Shanghai 200240, China
    dState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China
    eShanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Shanghai 201204, China
  • Received:2024-01-05 Accepted:2024-05-27 Online:2024-07-18 Published:2024-07-10
  • Contact: E-mail: xupengtao@sjtu.edu.cn (P. Xu), liuxi@sjtu.edu.cn (X. Liu), lwchen2018@sjtu.edu.cn (L. Chen).
  • About author:First author contact:

    1 Contributed equally to this work.

  • Supported by:
    National Key R&D Program of China(2021YFA1500300);National Key R&D Program of China(2022YFA1500146);National Key R&D Program of China(2021YFB3800300);National Natural Science Foundation of China(22072090);National Natural Science Foundation of China(22272106);National Natural Science Foundation of China(21991153);National Natural Science Foundation of China(21991150);National Natural Science Foundation of China(22372099)

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Abstract:

High-entropy alloy (HEA) catalysts exhibit enhanced hydrogen evolution reaction (HER) activity in water electrolysis, yet the understanding of their structure and active sites in reaction environments remains unclear. Here, we systematically investigated the HER activity and stability of PtPdRhRuCu/C through a combination of electrochemical measurements, in situ synchrotron radiation X-ray absorption spectroscopy (XAS) at the Cu K-edge and Pt L3-edge, and density functional theory (DFT) calculations. Uniformly sized PtPdRhRuCu HEA nanoparticles were prepared via a facile one-step solvothermal method. In situ XAS results revealed that the HEA nanoparticles maintained metallic states and a disordered arrangement of the overall structure at hydrogen evolution potential, implying the absence of the separated phases. Relying on multi-metal active sites, PtPdRhRuCu/C demonstrated a remarkably low overpotential of 23.3 mV at 10 mA cm-2 in alkaline HER, which is significantly lower than the overpotential observed in commercial Pt/C (50.3 mV), and achieving a mass activity 7.9 times that of Pt/C. DFT calculations show that the synergy of each metal site optimizes the dissociation energy barrier of water molecules. This study not only demonstrates the advancement of high-entropy alloys in electrocatalysis but also provides a comprehensive understanding of the structure-activity relationship of these unique catalysts through detailed characterizations. Our findings further contribute to the rational design and application of high-entropy alloy catalysts, specifically in HER.

Key words: Hydrogen evolution reaction, High-entropy alloy, In situ X-ray absorption spectroscopy, One-step solvothermal method, Lower overpotential