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Frustrated Lewis pair boosting photocatalytic antibacterial activity on PDI-bridged bimetallic UiO-66-NH2

Journal 2023 · IF 4 · 52(20): 6813-6822 · 发表于 2023 年 5 月 3 日
作者: Ruowen Liang,Shihui Wang,Yuzhou Xia,Ling Wu,Renkun Huang,Zhoujun He
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摘要

Designing frustrated Lewis pair (FLP)-structured photocatalysts is a new challenge in catalysis. In particular, the relationship between the active sites and photocatalytic charge transport mechanism over FLP-structured photocatalysts is still ill-defined. In this study, a novel perylene-3,4,9,10-tetracarboxylic diimide/UiO-66(Ti/Zr)–NH2 (denoted as PDI/TUZr) photocatalyst is successfully constructed using an ammoniation process. The PDI/TUZr heterojunction is equipped with a unique “Zr/Ti SBUs-ligand-PDI” FLP structure and exhibits remarkable catalytic FLP properties. In this “Zr/Ti SBUs-ligand-PDI” structure, the Zr/Ti bimetal centers and PDI serve as Lewis acid and base sites, respectively, and the C–N chemical bond provides a channel for electron transmission, and a bimetallic system facilitates electron transfer from excited ligand to Zr/Ti-SBUs nodes. These superior microstructural designs cooperate to promote substrate activation for photocatalytic antibacterial reactions. Accordingly, 2.2-fold enhancement is achieved in visible photocatalytic antibacterial activity on Staphylococcus aureus for 4%PDI/0.2TUZr composite compared with unadorned UZr. This study provides insights into the formation and carrier transfer behaviors of solid FLP on MOFs and illustrates a rational strategy for the construction of highly efficient photocatalysts.

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