Volume 19, Issue 32 2301178
Research Article

Electronic Structure Engineering of Pt Species over Pt/WO3 toward Highly Efficient Electrocatalytic Hydrogen Evolution

Xueliang Fan

Xueliang Fan

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433 China

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Cong Liu

Cong Liu

Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai, 200237 China

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Boxu Gao

Boxu Gao

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433 China

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He Li

He Li

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433 China

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Yahong Zhang

Yahong Zhang

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433 China

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Hongbin Zhang

Corresponding Author

Hongbin Zhang

Institute for Preservation of Chinese Ancient Books, Fudan University Library, Fudan University, Shanghai, 200433 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Qingsheng Gao

Corresponding Author

Qingsheng Gao

College of Chemistry and Materials Science, and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou, 510632 P. R. China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Xiaoming Cao

Corresponding Author

Xiaoming Cao

Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai, 200237 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Yi Tang

Corresponding Author

Yi Tang

Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433 China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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First published: 17 April 2023
Citations: 10

Abstract

Pt-based supported materials, a widely used electrocatalyst for hydrogen evolution reaction (HER), often experience unavoidable electron loss, resulting in a mismatching of electronic structure and HER behavior. Here, a Pt/WO3 catalyst consisting of Pt species strongly coupled with defective WO3 polycrystalline nanorods is rationally designed. The electronic structure engineering of Pt sites on WO3 can be systematically regulated, and so that the optimal electron-rich Pt sites on Pt/WO3-600 present an excellent HER activity with only 8 mV overpotential at 10 mA cm−2. Particularly, the mass activity reaches 7015 mA mg−1 at the overpotential of 50 mV, up to 26-fold higher than that of the commercial Pt/C. The combination of experimental and theoretical results demonstrates that the O vacancies of WO3 effectively mitigate the tendency of electron transfer from Pt sites to WO3, so that the d-band center could reach an appropriate level relative to Fermi level, endowing it with a suitable Δ G H $\Delta {G_{{{\rm{H}}^ * }}}$ . This work identifies the influence of the electronic structure on catalytic activity.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available on request from the corresponding author. The data are not publicly available due to privacy or ethical restrictions.

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