Regulating Electronic Structure of Single-Atom Catalysts toward Efficient Bifunctional Oxygen Electrocatalysis

Ji, Jiapeng; Wu, Lei; Zhou, Shiyu Y.; Qiu, Tong; Li, Zeheng; Wang, Liguang; Zhang, Liang; Ma, Lu; Ling, Min; Zhou, Shaodong; Liang, Chengdu

doi:10.1002/smtd.202101511

Title: Regulating Electronic Structure of Single-Atom Catalysts toward Efficient Bifunctional Oxygen Electrocatalysis

Journal Article · 16 February 2022 · Small Methods

DOI: https://doi.org/10.1002/smtd.202101511 · OSTI ID:1890211

^[1]; Wu, Lei ^[1]; Zhou, Shiyu Y. ^[1]; Qiu, Tong ^[1]; Li, Zeheng ^[1]; Wang, Liguang ^[2]; Zhang, Liang ^[3]; Ma, Lu ^[4];

^[2]; Zhou, Shaodong ^[1]; Liang, Chengdu ^[1]

Zhejiang University, Hangzhou (China)
Zhejiang University, Hangzhou (China); Institute of Zhejiang University-Quzhou (China)
Soochow University, Suzhou (China)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

We report electronic structure of single-atom catalysts (SACs) is critical for bifunctional oxygen electrocatalysis by adjusting the binding energy in oxygen-containing intermediates. However, the regulation of electronic structure has always been a challenge to improve catalytic reactivity. Herein, by introducing a heterogenous metal, the electronic structure through a direct bonding interaction to the active center atom is effectively adjusted. Partial charge transfer between the two atoms optimizes the binding energy of intermediates and reducing the energy barrier of the catalytic reaction. Theoretical calculations confirm these effects and the uniform distribution of 3d orbitals, leading to the improvement of bifunctional oxygen electrocatalytic reactivity. Benefiting from these attributes, the as-constructed bifunctional catalyst enables outstanding electrocatalytic performances in both oxygen reduction and hydrogen oxidation in various energy storage systems. The generality and expandability of this strategy is demonstrated by further successful development of other dual-metal catalysts systems with various active metals.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Key R&D Program of China; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); Zhejiang University

Grant/Contract Number:: SC0012704

OSTI ID:: 1890211

Report Number(s):: BNL-223517-2022-JAAM

Journal Information:: Small Methods, Journal Name: Small Methods Journal Issue: 4 Vol. 6; ISSN 2366-9608

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
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electronic structure regulation
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Title: Regulating Electronic Structure of Single-Atom Catalysts toward Efficient Bifunctional Oxygen Electrocatalysis

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