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A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

Author

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  • Jiayuan Li

    (Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University)

  • Jun Hu

    (School of Chemical Engineering, Northwest University)

  • Mingkai Zhang

    (Frontier Institute of Science and Technology, Xi’an Jiaotong University)

  • Wangyan Gou

    (Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University)

  • Sai Zhang

    (Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University)

  • Zhong Chen

    (School of Materials Science and Engineering, Nanyang Technological University)

  • Yongquan Qu

    (Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
    Frontier Institute of Science and Technology, Xi’an Jiaotong University)

  • Yuanyuan Ma

    (Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University)

Abstract

Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.

Suggested Citation

  • Jiayuan Li & Jun Hu & Mingkai Zhang & Wangyan Gou & Sai Zhang & Zhong Chen & Yongquan Qu & Yuanyuan Ma, 2021. "A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23750-4
    DOI: 10.1038/s41467-021-23750-4
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    Cited by:

    1. Bingxing Zhang & Baohua Zhang & Guoqiang Zhao & Jianmei Wang & Danqing Liu & Yaping Chen & Lixue Xia & Mingxia Gao & Yongfeng Liu & Wenping Sun & Hongge Pan, 2022. "Atomically dispersed chromium coordinated with hydroxyl clusters enabling efficient hydrogen oxidation on ruthenium," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. Jiadong Chen & Chunhong Chen & Minkai Qin & Ben Li & Binbin Lin & Qing Mao & Hongbin Yang & Bin Liu & Yong Wang, 2022. "Reversible hydrogen spillover in Ru-WO3-x enhances hydrogen evolution activity in neutral pH water splitting," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Liu, Haobo & Zhang, Yuqi & Ge, Riyue & Cairney, Julie M. & Zheng, Rongkun & Khan, Aslam & Li, Sean & Liu, Bin & Dai, Liming & Li, Wenxian, 2023. "Tailoring the electronic structure of Ni5P4/Ni2P catalyst by Co2P for efficient overall water electrolysis," Applied Energy, Elsevier, vol. 349(C).
    4. Zhe Wang & Chunpeng Wang & Shanjun Mao & Bing Lu & Yuzhuo Chen & Xie Zhang & Zhirong Chen & Yong Wang, 2022. "Decoupling the electronic and geometric effects of Pt catalysts in selective hydrogenation reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    5. Jie Dai & Yinlong Zhu & Yu Chen & Xue Wen & Mingce Long & Xinhao Wu & Zhiwei Hu & Daqin Guan & Xixi Wang & Chuan Zhou & Qian Lin & Yifei Sun & Shih-Chang Weng & Huanting Wang & Wei Zhou & Zongping Sha, 2022. "Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    6. Zhenglong Fan & Fan Liao & Yujin Ji & Yang Liu & Hui Huang & Dan Wang & Kui Yin & Haiwei Yang & Mengjie Ma & Wenxiang Zhu & Meng Wang & Zhenhui Kang & Youyong Li & Mingwang Shao & Zhiwei Hu & Qi Shao, 2022. "Coupling of nanocrystal hexagonal array and two-dimensional metastable substrate boosts H2-production," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Sheng Zhao & Sung-Fu Hung & Liming Deng & Wen-Jing Zeng & Tian Xiao & Shaoxiong Li & Chun-Han Kuo & Han-Yi Chen & Feng Hu & Shengjie Peng, 2024. "Constructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    8. Zhi Wen Chen & Jian Li & Pengfei Ou & Jianan Erick Huang & Zi Wen & LiXin Chen & Xue Yao & GuangMing Cai & Chun Cheng Yang & Chandra Veer Singh & Qing Jiang, 2024. "Unusual Sabatier principle on high entropy alloy catalysts for hydrogen evolution reactions," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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