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

Jiayuan Li, Jun Hu (), Mingkai Zhang, Wangyan Gou, Sai Zhang, Zhong Chen, Yongquan Qu () and Yuanyuan Ma ()
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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
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

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-23750-4

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