Issue 20, 2024

Synergism between metal single-atom sites and S-vacant two-dimensional nanosheets for efficient hydrogen evolution uncovered by density functional theory and machine learning

Abstract

Efficient electrocatalysts for the hydrogen evolution reaction (HER) are the key to hydrogen-electricity energy conversion. Leveraging density functional theory and machine learning, we herein reveal the synergism between metal single atoms (M-SAs) and S-vacant two-dimensional (2D) MnPS3 nanosheets (Sv-MnPS3). Specifically, M-SAs occupy S-vacancies and activate the neighboring S sites as new active sites for the HER. In turn, Sv-MnPS3 improves the ability of metal-SAs for water dissociation by modulating their magnetic moments. During the HER, H* is generated on metal-SAs and then migrates to neighboring S sites on which H2 is produced, representing catalytic synergism via hydrogen spillover. Among the M1/Sv-MnPS3 candidates, Pd1/Sv-MnPS3 possesses an optimal ΔGH* of 0.01 eV and is both thermodynamically and electrochemically stable. Therefore, the synergism between Pd1 and Sv-MnPS3 enables Pd1/Sv-MnPS3 to be active and durable for the HER. This work provides insights into how to design and understand confined metal-SAs in 2D materials for efficient electrocatalysis.

Graphical abstract: Synergism between metal single-atom sites and S-vacant two-dimensional nanosheets for efficient hydrogen evolution uncovered by density functional theory and machine learning

Supplementary files

Article information

Article type
Research Article
Submitted
09 Jul 2024
Accepted
04 Sep 2024
First published
18 Sep 2024

Inorg. Chem. Front., 2024,11, 7008-7017

Synergism between metal single-atom sites and S-vacant two-dimensional nanosheets for efficient hydrogen evolution uncovered by density functional theory and machine learning

X. Li, D. Jiao, J. Zhao and X. Zhao, Inorg. Chem. Front., 2024, 11, 7008 DOI: 10.1039/D4QI01723D

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