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Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis.


ABSTRACT: The unsatisfactory catalytic activity of nanozymes owing to their inefficient electron transfer (ET) is the major challenge in biomimetic catalysis-related biomedical applications. Inspired by the photoelectron transfers in natural photoenzymes, we herein report a photonanozyme of single-atom Ru anchored on metal-organic frameworks (UiO-67-Ru) for achieving photoenhanced peroxidase (POD)-like activity. We demonstrate that the atomically dispersed Ru sites can realize high photoelectric conversion efficiency, superior POD-like activity (7.0-fold photoactivity enhancement relative to that of UiO-67), and good catalytic specificity. Both in situ experiments and theoretical calculations reveal that photoelectrons follow the cofactor-mediated ET process of enzymes to promote the production of active intermediates and the release of products, demonstrating more favorable thermodynamics and kinetics in H2O2 reduction. Taking advantage of the unique interaction of the Zr-O-P bond, we establish a UiO-67-Ru-based immunoassay platform for the photoenhanced detection of organophosphorus pesticides.

SUBMITTER: Xu W 

PROVIDER: S-EPMC10214184 | biostudies-literature | 2023 May

REPOSITORIES: biostudies-literature

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Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis.

Xu Weiqing W   Zhong Hong H   Wu Yu Y   Qin Ying Y   Jiao Lei L   Sha Meng M   Su Rina R   Tang Yinjun Y   Zheng Lirong L   Hu Liuyong L   Zhang Shipeng S   Beckman Scott P SP   Gu Wenling W   Yang Yong Y   Guo Shaojun S   Zhu Chengzhou C  

Proceedings of the National Academy of Sciences of the United States of America 20230515 21


The unsatisfactory catalytic activity of nanozymes owing to their inefficient electron transfer (ET) is the major challenge in biomimetic catalysis-related biomedical applications. Inspired by the photoelectron transfers in natural photoenzymes, we herein report a photonanozyme of single-atom Ru anchored on metal-organic frameworks (UiO-67-Ru) for achieving photoenhanced peroxidase (POD)-like activity. We demonstrate that the atomically dispersed Ru sites can realize high photoelectric conversio  ...[more]

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