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Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts

Jiace Hao, Zechao Zhuang, Kecheng Cao, Guohua Gao, Chan Wang, Feili Lai, Shuanglong Lu, Piming Ma, Weifu Dong, Tianxi Liu, Mingliang Du and Han Zhu (zhysw@jiangnan.edu.cn)
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Jiace Hao: Jiangnan University
Zechao Zhuang: Tsinghua University
Kecheng Cao: ShanghaiTech University
Guohua Gao: Tongji University
Chan Wang: Jiangnan University
Feili Lai: KU Leuven
Shuanglong Lu: Jiangnan University
Piming Ma: Jiangnan University
Weifu Dong: Jiangnan University
Tianxi Liu: Jiangnan University
Mingliang Du: Jiangnan University
Han Zhu: Jiangnan University

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

Abstract: Abstract High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH* and H* intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.

Date: 2022
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DOI: 10.1038/s41467-022-30379-4

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