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Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis

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 anc...

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Detalles Bibliográficos
Autores principales: Xu, Weiqing, Zhong, Hong, Wu, Yu, Qin, Ying, Jiao, Lei, Sha, Meng, Su, Rina, Tang, Yinjun, Zheng, Lirong, Hu, Liuyong, Zhang, Shipeng, Beckman, Scott P., Gu, Wenling, Yang, Yong, Guo, Shaojun, Zhu, Chengzhou
Formato: Online Artículo Texto
Lenguaje:English
Publicado: National Academy of Sciences 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10214184/
https://www.ncbi.nlm.nih.gov/pubmed/37186847
http://dx.doi.org/10.1073/pnas.2220315120
Descripción
Sumario: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 H(2)O(2) 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.