Authors
Chang Liu, Wei Geng, Yuxuan Tan, Jiayang Shi, Faheem Abbas, Yanan Fan, Sha Zhang, Haili Song, Yu Zhang, Duidui Zhang, Chen Chen, Cheng-Xia Chen, Cheng-Yong Su, Yongge Wei
Published in
Angewandte Chemie (International ed. in English). Pages e8540353. Aug 05, 2026. Epub Aug 05, 2026.
Abstract
Photocatalytic CO2 reduction to methane (CH4) is highly desirable but severely hindered by sluggish multiple proton-coupled electron transfer (MPCET) kinetics and poor product selectivity. In this study, we report a novel one-dimensional (1D) copper coordination polymer, termed Cu-PMo12, featuring single-site Cu centers periodically bridged by Keggin-type {PMo12} clusters. Comprehensive experimental and theoretical studies reveal a synergistic mechanism governed by static electronic modulation and dynamic photoactivation. In the ground state, {PMo12} acts as an electron acceptor, withdrawing electrons from Cu sites to upshift the Cu d-band center, thereby strengthening the binding affinity toward intermediates. Under visible-light irradiation, {PMo12} functions as a photosensitizer and a light-switchable "electron pump", directionally injecting photogenerated electrons to Cu sites to dynamically maintain highly active Cu(I) species for the subsequent MPCET process. Consequently, Cu-PMo12 achieves an exceptional CH4 evolution rate of 70.5 µmol gCu - 1 h- 1 with near-unity selectivity (∼100%) and excellent durability. This work highlights precise microenvironment engineering via polyoxometalate-metal integration and provides a paradigm for designing light-driven "electron pump" systems for challenging multi-electron catalytic transformations.
PMID:
42554445
Bibliographic data and abstract were imported from PubMed on 05 Aug 2026.
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