Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis

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 and Zongping Shao ()
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Jie Dai: Nanjing Tech University
Yinlong Zhu: Monash University
Yu Chen: Monash University
Xue Wen: Shanghai Jiao Tong University
Mingce Long: Shanghai Jiao Tong University
Xinhao Wu: Nanjing Tech University
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Daqin Guan: Nanjing Tech University
Xixi Wang: Nanjing Tech University
Chuan Zhou: Nanjing Tech University
Qian Lin: Monash University
Yifei Sun: College of Energy, Xiamen University
Shih-Chang Weng: National Synchrotron Radiation Research Center
Huanting Wang: Monash University
Wei Zhou: Nanjing Tech University
Zongping Shao: Nanjing Tech University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Improving the catalytic efficiency of platinum for the hydrogen evolution reaction is valuable for water splitting technologies. Hydrogen spillover has emerged as a new strategy in designing binary-component Pt/support electrocatalysts. However, such binary catalysts often suffer from a long reaction pathway, undesirable interfacial barrier, and complicated synthetic processes. Here we report a single-phase complex oxide La2Sr2PtO7+δ as a high-performance hydrogen evolution electrocatalyst in acidic media utilizing an atomic-scale hydrogen spillover effect between multifunctional catalytic sites. With insights from comprehensive experiments and theoretical calculations, the overall hydrogen evolution pathway proceeds along three steps: fast proton adsorption on O site, facile hydrogen migration from O site to Pt site via thermoneutral La-Pt bridge site serving as the mediator, and favorable H2 desorption on Pt site. Benefiting from this catalytic process, the resulting La2Sr2PtO7+δ exhibits a low overpotential of 13 mV at 10 mA cm−2, a small Tafel slope of 22 mV dec−1, an enhanced intrinsic activity, and a greater durability than commercial Pt black catalyst.

Date: 2022
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DOI: 10.1038/s41467-022-28843-2

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