Harnessing Hydrogen Spillover by Lattice Strain for Enhanced Photocatalytic Hydrogen Evolution of ZnIn2S4

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-01-25 DOI:10.1021/acscatal.4c07308

Fan Gao, Wen-Gang Cui, Xinqiang Wang, Zhenglong Li, Yongchang Chen, Zichao Shen, Ke Wang, Yong Gao, Jian Miao, Yaxiong Yang, Jian Chen, Shaohua Shen, Hongge Pan

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引用次数: 0

Abstract

Hydrogen spillover has been believed to play an essential role in the reaction path in photocatalysis, yet its rational regulation remains a considerable challenge for the design of highly efficient photocatalysts. Herein, hydrogen spillover can be well regulated at ZnIn₂S₄ with surface decorated by cubic α-MoC_1–x quantum dots (QDs) with different lattice strain (ZIS/QDs). With the increasing lattice strain of α-MoC_1–x, the composite shows first increased and then decreased photocatalytic hydrogen evolution (PHE). Spectroscopic characterizations and calculation analysis indicate that PHE performance of ZIS/QDs is highly corelated with hydrogen spillover rather than charge transfer process. Further systematic investigations suggest that compressive lattice strain uplifts the Fermi level of α-MoC_1–x and optimizes the interfacial spillover barrier between α-MoC_1–x and ZnIn₂S₄, achieving well-manipulated hydrogen spillover and enhanced PHE performance. This work demonstrates a general design from the perspective of lattice strain to harness hydrogen spillover effect in heterogeneous interface for hydrogen generation.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.