Constructing Molecular Junctions with High-Spin Metal Sites in POMOFs to Trigger Heteropoly Blue States for Photocatalytic H 2  Production

Sun, Weize; Zhao, Bo; Gómez‐García, Carlos J.; Pang, Haijun; Lang, Zhongling; Ma, Huiyuan; Wang, Xinming; Yang, Guixin; Au, Chi‐Ming; Yu, Wing‐Yiu

doi:10.1021/acscatal.5c01006

articleACS CatalysisApr 23, 2025GREEN OA

Constructing Molecular Junctions with High-Spin Metal Sites in POMOFs to Trigger Heteropoly Blue States for Photocatalytic H 2 Production

WSWeize Sun BZBo Zhao CJCarlos J. Gómez‐García HPHaijun Pang ZLZhongling Lang

Harbin University of Science and Technology · Northeast Normal University · +2 more institutions

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Abstract

The spin state of metal atoms may play a key role in the photocatalytic hydrogen evolution reaction (HER) of polyoxometalate (POM)-based catalysts. Herein, we construct two POM-based metal–organic frameworks (POMOFs) with molecular junction structures by integrating a metal–organic framework structure including high-spin state active Co or Ni sites with [GeW12O40]4– (GeW12) POM. These structures have a fast electron transfer channel, in which the electronic structures of the high-spin metal centers may determine whether the POM can produce reduced POM (heteropoly blue, HPB), leading to enhanced HER activity. Upon photoexcitation, the CoII high-spin state has a vacant in the t2g orbital, which transfers…

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Topics & keywords

Topics

Keywords

Photocatalysis
Catalysis
Metal
Materials science
Spin (aerodynamics)
Photochemistry
Nanotechnology
Chemistry

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