Volume 58, Issue 49 pp. 17709-17717
Research Article

Surface-Electron Coupling for Efficient Hydrogen Evolution

Weiwei Fu

Weiwei Fu

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

These authors contributed equally to this work.

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Yanwei Wang

Yanwei Wang

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

These authors contributed equally to this work.

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Jisong Hu

Jisong Hu

School of Science, Hubei University of Technology, Wuhan, 430068 P. R. China

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Huijuan Zhang

Huijuan Zhang

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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Ping Luo

Ping Luo

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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Fang Sun

Fang Sun

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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Xinguo Ma

Xinguo Ma

School of Science, Hubei University of Technology, Wuhan, 430068 P. R. China

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Zhengyong Huang

Zhengyong Huang

The School of Electrical Engineering, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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Jian Li

Jian Li

The School of Electrical Engineering, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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Zaiping Guo

Corresponding Author

Zaiping Guo

Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Innovation Campus, North Wollongong, NSW, 2500 Australia

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Yu Wang

Corresponding Author

Yu Wang

The School of Chemistry and Chemical Engineering, State Key Laboratory of Power Transmission Equipment & System Security and New Technology, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

The School of Electrical Engineering, Chongqing University, 174 Shazheng Street, Shapingba District, Chongqing City, 400044 P. R. China

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First published: 02 September 2019
Citations: 49

Graphical Abstract

Small modifications have N effect: The controllable modification of graphene/V8C7 heterostructures by nitrogen is reported. Due to changes in the electronic structure of the different parts of the modified heterostructure, it displays an exceptional alkaline hydrogen-evolution capability, the most efficient alkaline hydrogen-evolution catalysis among transition-metal carbides reported thus far.

Abstract

Maximizing the activity of materials towards the alkaline hydrogen evolution reaction while maintaining their structural stability under realistic working conditions remains an area of active research. Herein, we report the first controllable surface modification of graphene(G)/V8C7 heterostructures by nitrogen. Because the introduced N atoms couple electronically with V atoms, the V sites can reduce the energy barrier for water adsorption and dissociation. Investigation of the multi-regional synergistic catalysis on N-modified G/V8C7 by experimental observations and density-functional-theory calculations reveals that the increase of electron density on the epitaxial graphene enable it to become favorable for H* adsorption and the subsequent reaction with another H2O molecule. This work extends the range of surface-engineering approaches to optimize the intrinsic properties of materials and could be generalized to the surface modification of other transition-metal carbides.

Conflict of interest

The authors declare no conflict of interest.

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