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Pt-Co single atom alloy catalysts: Accelerated water dissociation and hydrogen evolution by strain regulation

Journal of Energy Chemistry 2022年第6期31卷 44-53,I0002页

作者： rendian wan Mi Luo Jingbo Wen Shilong Liu Xiongwu Kang Yong Tian School of Pharmacy Guangdong Pharmaceutical UniversityGuangzhou 510006GuangdongChina New Energy Research Institute School of Environment and EnergySouth China University of TechnologyHigher Education Mega CenterGuangzhou 510006GuangdongChina

The alkaline hydrogen evolution reaction(HER) on Pt-based catalysts is largely limited by the slow water dissociation kinetics. Pt-based single atom alloy catalysts(SAAC) with water dissociation sites have been demonstrated as excellent alkaline HER catalysts. However, the regulation of their activity and stability at the atomic scale is still a great challenge. Herein, the kinetic and stability issues are successfully resolved via engineering the electronic structure of Pt-Co SAAC by Au-induced tensile strain. The atomic dispersion of Co into the Pt shell was confirmed by extended X-ray absorption fine structure and the electronic structure and catalytic HER performance was modulated by the tensile strain induced by the Pt shell thickness. An inverse volcano-type relation between HER activity and surface strain was found.Density functional theory(DFT) calculations reveal that the Au-induced tensile strain on Pt-Co shell can not only boost the adsorption and dissociation kinetics of water at Co site by upshifting the dband and promoting the electron transfer, but also downshift the d-band center of Pt in Pt-Co shell, leading to optimized H* adsorption/desorption. The champion catalyst provides an overpotential of only 14 m V at the current density of 10 mA cm^(-2). This work not only provides an effective strategy for the construction of single-atom alloy electrocatalysts for high performance toward alkaline HER but also sheds light on the understanding of the reaction mechanism at the atomic level.

关键词： Hydrogen evolution reaction Single atom alloy Strain DFT calculation d-band

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