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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...
Autores principales: | , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2023
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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 |
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author | 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 |
author_facet | 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 |
author_sort | Xu, Weiqing |
collection | PubMed |
description | 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. |
format | Online Article Text |
id | pubmed-10214184 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-102141842023-11-15 Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis 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 Proc Natl Acad Sci U S A Physical Sciences 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. National Academy of Sciences 2023-05-15 2023-05-23 /pmc/articles/PMC10214184/ /pubmed/37186847 http://dx.doi.org/10.1073/pnas.2220315120 Text en Copyright © 2023 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) . |
spellingShingle | Physical Sciences 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 Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title | Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title_full | Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title_fullStr | Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title_full_unstemmed | Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title_short | Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis |
title_sort | photoexcited ru single-atomic sites for efficient biomimetic redox catalysis |
topic | Physical Sciences |
url | 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 |
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