Modulating Built-In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Lingling Zhai; Xiaojie She; Lyuchao Zhuang; Yanyong Li; Ran Ding; Xuyun Guo; Yongqi Zhang; Ye Zhu; Kun Xu; Hong Jin Fan; Shu Ping Lau

doi:10.1002/anie.202116057

Modulating Built-In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Lingling Zhai, Xiaojie She, Lyuchao Zhuang, Yanyong Li, Ran Ding, Xuyun Guo, Yongqi Zhang, Ye Zhu, Kun Xu, Hong Jin Fan, Shu Ping Lau

Research output: Journal article publication › Journal article › Academic research › peer-review

210 Citations (Scopus)

Abstract

Work function strongly impacts the surficial charge distribution, especially for metal-support electrocatalysts when a built-in electric field (BEF) is constructed. Therefore, studying the correlation between work function and BEF is crucial for understanding the intrinsic reaction mechanism. Herein, we present a Pt@CoO_x electrocatalyst with a large work function difference (ΔΦ) and strong BEF, which shows outstanding hydrogen evolution activity in a neutral medium with a 4.5-fold mass activity higher than 20 % Pt/C. Both experimental and theoretical results confirm the interfacial charge redistribution induced by the strong BEF, thus subtly optimizing hydrogen and hydroxide adsorption energy. This work not only provides fresh insights into the neutral hydrogen evolution mechanism but also proposes new design principles toward efficient electrocatalysts for hydrogen production in a neutral medium.

Original language	English
Article number	e202116057
Journal	Angewandte Chemie - International Edition
Volume	61
Issue number	14
DOIs	https://doi.org/10.1002/anie.202116057
Publication status	Published - 28 Mar 2022

Keywords

Built-in Electric Field
Electrocatalysis
Hydrogen Evolution Reaction
Metal-Support Interaction
Work Function

ASJC Scopus subject areas

Catalysis
General Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

More information

10.1002/anie.202116057

http://hdl.handle.net/10397/94025

Cite this

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title = "Modulating Built-In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media",

abstract = "Work function strongly impacts the surficial charge distribution, especially for metal-support electrocatalysts when a built-in electric field (BEF) is constructed. Therefore, studying the correlation between work function and BEF is crucial for understanding the intrinsic reaction mechanism. Herein, we present a Pt@CoOx electrocatalyst with a large work function difference (ΔΦ) and strong BEF, which shows outstanding hydrogen evolution activity in a neutral medium with a 4.5-fold mass activity higher than 20 % Pt/C. Both experimental and theoretical results confirm the interfacial charge redistribution induced by the strong BEF, thus subtly optimizing hydrogen and hydroxide adsorption energy. This work not only provides fresh insights into the neutral hydrogen evolution mechanism but also proposes new design principles toward efficient electrocatalysts for hydrogen production in a neutral medium.",

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note = "Funding Information: This work was financially supported by the Research Grants Council of Hong Kong (PolyU 253009/18P) and the Hong Kong Polytechnic University (1‐ZVGH). H.J.F. thanks the financial support from Agency for Science, Technology, and Research (A*STAR), Singapore by AME Individual Research Grants (A1983c0026). Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH",

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AU - Zhai, Lingling

AU - She, Xiaojie

AU - Zhuang, Lyuchao

AU - Li, Yanyong

AU - Ding, Ran

AU - Guo, Xuyun

AU - Zhang, Yongqi

AU - Zhu, Ye

AU - Xu, Kun

AU - Fan, Hong Jin

AU - Lau, Shu Ping

N1 - Funding Information: This work was financially supported by the Research Grants Council of Hong Kong (PolyU 253009/18P) and the Hong Kong Polytechnic University (1‐ZVGH). H.J.F. thanks the financial support from Agency for Science, Technology, and Research (A*STAR), Singapore by AME Individual Research Grants (A1983c0026). Publisher Copyright: © 2022 Wiley-VCH GmbH

PY - 2022/3/28

Y1 - 2022/3/28

N2 - Work function strongly impacts the surficial charge distribution, especially for metal-support electrocatalysts when a built-in electric field (BEF) is constructed. Therefore, studying the correlation between work function and BEF is crucial for understanding the intrinsic reaction mechanism. Herein, we present a Pt@CoOx electrocatalyst with a large work function difference (ΔΦ) and strong BEF, which shows outstanding hydrogen evolution activity in a neutral medium with a 4.5-fold mass activity higher than 20 % Pt/C. Both experimental and theoretical results confirm the interfacial charge redistribution induced by the strong BEF, thus subtly optimizing hydrogen and hydroxide adsorption energy. This work not only provides fresh insights into the neutral hydrogen evolution mechanism but also proposes new design principles toward efficient electrocatalysts for hydrogen production in a neutral medium.

AB - Work function strongly impacts the surficial charge distribution, especially for metal-support electrocatalysts when a built-in electric field (BEF) is constructed. Therefore, studying the correlation between work function and BEF is crucial for understanding the intrinsic reaction mechanism. Herein, we present a Pt@CoOx electrocatalyst with a large work function difference (ΔΦ) and strong BEF, which shows outstanding hydrogen evolution activity in a neutral medium with a 4.5-fold mass activity higher than 20 % Pt/C. Both experimental and theoretical results confirm the interfacial charge redistribution induced by the strong BEF, thus subtly optimizing hydrogen and hydroxide adsorption energy. This work not only provides fresh insights into the neutral hydrogen evolution mechanism but also proposes new design principles toward efficient electrocatalysts for hydrogen production in a neutral medium.

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KW - Electrocatalysis

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KW - Metal-Support Interaction

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Modulating Built-In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Abstract

Keywords

ASJC Scopus subject areas

UN SDGs

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