Improving Alkaline Hydrogen Oxidation through Dynamic Lattice Hydrogen Migration in Pd@Pt Core‐Shell Electrocatalysts

Author:

Zhao Tonghui1,Li Mengting2,Xiao Dongdong3,Yang Xiaoju1,An Lulu1,Deng Zhiping1,Shen Tao1,Gong Mingxing1,Chen Yi1,Liu Hongfang1,Feng Ligang4,Yang Xuan1,Li Li2,Wang Deli1ORCID

Affiliation:

1. Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 P. R. China

2. The State Key Laboratory of Power Transmission Equipment & System Security and New Technology Chongqing Key Laboratory of Chemical Process for Clean Energy and Resource Utilization School of Chemistry and Chemical Engineering Chongqing University Chongqing 400044 P. R. China

3. Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 P. R. China

4. School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 P. R. China

Abstract

AbstractTracking the trajectory of hydrogen intermediates during hydrogen electro‐catalysis is beneficial for designing synergetic multi‐component catalysts with division of chemical labor. Herein, we demonstrate a novel dynamic lattice hydrogen (LH) migration mechanism that leads to two orders of magnitude increase in the alkaline hydrogen oxidation reaction (HOR) activity on Pd@Pt over pure Pd, even ≈31.8 times mass activity enhancement than commercial Pt. Specifically, the polarization‐driven electrochemical hydrogenation process from Pd@Pt to PdHx@Pt by incorporating LH allows more surface vacancy Pt sites to increase the surface H coverage. The inverse dehydrogenation process makes PdHx as an H reservoir, providing LH migrates to the surface of Pt and participates in the HOR. Meanwhile, the formation of PdHx induces electronic effect, lowering the energy barrier of rate‐determining Volmer step, thus resulting in the HOR kinetics on Pd@Pt being proportional to the LH concentration in the in situ formed PdHx@Pt. Moreover, this dynamic catalysis mechanism would open up the catalysts scope for hydrogen electro‐catalysis.

Funder

National Natural Science Foundation of China

Fundamental Research Funds for the Central Universities

China Postdoctoral Science Foundation

Natural Science Foundation of Beijing Municipality

Publisher

Wiley

Subject

General Medicine

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