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Synergistic structural and electronic regulation of copper-based metal-covalent organic frameworks for improving bifunctional photocatalysis
Yan Sun, Yafei Qian, Ning An, Jingwei Huang, Houde She, Lei Wang*, Qizhao Wang*
https://doi.org/10.1016/j.cjsc.2026.101079
Photocatalysis; Metal-covalent organic framework; H2O2 photosynthesis; Carbon dioxide reduction
ABSTRACT
Photocatalytic technology is an effective approach to address energy shortages and environmental problems. However, developing efficient and stable multifunctional photocatalysts remains a challenging task. In this study, two metal-covalent organic frameworks (MCOFs) were synthesized using a trinuclear copper cluster as the electron-rich node: TAPT-MCOF with a [3+3] configuration and Dip-MCOF with a [3+2] configuration. In the absence of sacrificial agent, TAPT-MCOF exhibits improved visible-light-driven photocatalytic performance in both hydrogen peroxide (H2O2) synthesis and carbon dioxide (CO2) reduction. The H2O2 production rate is 261.8 μmol g-1 h-1, about 2.4 times that of Dip-MCOF. The reaction rate for CO2 reduction is also higher than that of Dip-MCOF. The enhanced behavior originates from two synergistic effects: (ⅰ) the specific surface area of TAPT-MCOF in the [3+3] configuration affords favored transport channels for efficient mass migration, including the reactants and products; and (ⅱ) the triazine group with electron-deficient property (EDP) and the trinuclear copper (Cu3Py) cluster with electron-rich property (ERP) in TAPT-MCOF create a highly intensified local asymmetric charge distribution, effectively promoting the photogenerated electron-hole separation. This finding provides guidance for designing efficient bifunctional photocatalysts by leveraging the dual structure regulation of porous frameworks.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 闽ICP备2022002645号-1