Issue 14, 2024

Hierarchically stabilized Pt single-atom catalysts induced by an atomic substitution strategy for an efficient hydrogen evolution reaction

Abstract

Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER). Herein, we constructed a hierarchical stabilization system of Pt single-atoms via defect substitution using the polyoxometalate (POM) (NH4)4[ZnMo6O24H6] (ZnMo6) as a template. The well-defined structure of ZnMo6 led to precise local Zn sublimation during the formation of Mo2C, which was converted from the Mo6 ring in situ. The localized defect provides a well-defined Mo(C)–Pt–N coordination environment to trap Pt single-atoms. The obtained single-atom catalyst (PtSA@Mo2C@NC) exhibited a superior and stable electrochemical HER performance with an unprecedented mass activity of 75.21 A mgPt−1 in 0.5 M H2SO4. In-depth theoretical calculation analysis revealed that Mo(C)–Pt–N coordination provides a moderated charge state and low d-band center of the Pt site, thus significantly promoting proton adsorption and H2 desorption. This work demonstrates a promising single-atom stabilization strategy for constructing high-performance HER electrocatalysts through the precise modulation of a three-dimensional chemical environment.

Graphical abstract: Hierarchically stabilized Pt single-atom catalysts induced by an atomic substitution strategy for an efficient hydrogen evolution reaction

Supplementary files

Article information

Article type
Paper
Submitted
20 Dec 2023
Accepted
29 May 2024
First published
18 Jun 2024

Energy Environ. Sci., 2024,17, 5227-5240

Hierarchically stabilized Pt single-atom catalysts induced by an atomic substitution strategy for an efficient hydrogen evolution reaction

C. Yue, C. Feng, G. Sun, N. Liu, H. Hao, W. Bao, X. Zhang, F. Sun, C. Zhang, J. Bi, Y. Zhou, H. Chen, Y. Pan, D. Sun and Y. Lu, Energy Environ. Sci., 2024, 17, 5227 DOI: 10.1039/D3EE04457B

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