Volume 20, Issue 31 2311221
Research Article

Boosting Efficient Alkaline Hydrogen Evolution Reaction of CoFe-Layered Double Hydroxides Nanosheets via Co-Coordination Mechanism of W-Doping and Oxygen Defect Engineering

Shaohong Wang

Shaohong Wang

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Jing Wu

Jing Wu

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Yin Xu

Yin Xu

Department of Environment, College of Environment and Resources, Xiangtan University, Xiangtan, Hunan, 411105 P. R. China

Hunan Key Lab for Environmental Behavior of New Pollutants and Control Principle, Xiangtan, Hunan, 411105 P. R. China

Search for more papers by this author
Dandan Liang

Dandan Liang

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Da Li

Da Li

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Dahong Chen

Dahong Chen

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Guohong Liu

Guohong Liu

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

Search for more papers by this author
Yujie Feng

Corresponding Author

Yujie Feng

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, No. 73 Huanghe Road, Nangang District, Harbin, 150090 P. R. China

E-mail: [email protected]

Search for more papers by this author
First published: 11 March 2024
Citations: 20

Abstract

While surface defects and heteroatom doping exhibit promising potential in augmenting the electrocatalytic hydrogen evolution reaction (HER), their performance remains unable to rival that of the costly Pt-based catalysts. Yet, the concurrent modification of catalysts by integrating both approaches stands as a promising strategy to effectively address the aforementioned limitation. In this work, tungsten dopants are introduced into self-supported CoFe-layered double hydroxides (LDH) on nickel foam using a hydrothermal method, and oxygen vacancies (Ov) are further introduced through calcination. The analysis results demonstrated that tungsten doping reduces the Ov formation energy of CoFeW-LDH. The Ov acted as oxophilic sites, facilitating water adsorption and dissociation, and reducing the barrier for cleaving HO─H bonds from 0.64 to 0.14 eV. Additionally, Ov regulated the electronic structure of CoFeW-LDH to endow optimized hydrogen binding ability on tungsten atoms, thereby accelerating alkaline Volmer and Heyrovsky reaction kinetics. Specifically, the abundance of Ov induced a transition of tungsten from a six-coordinated to highly active four-coordinated structure, which becomes the active site for HER. Consequently, an ultra-low overpotential of 41 mV at 10 mA cm−2, and a low Tafel slope of 35 mV dec−1 are achieved. These findings offer crucial insights for the design of efficient HER electrocatalysts.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.