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

Authors :
Weiqing Xu
Hong Zhong
Yu Wu
Ying Qin
Lei Jiao
Meng Sha
Rina Su
Yinjun Tang
Lirong Zheng
Liuyong Hu
Shipeng Zhang
Beckman, Scott P.
Wenling Gu
Yong Yang
Shaojun Guo
Chengzhou Zhu
Source :
Proceedings of the National Academy of Sciences of the United States of America. 5/23/2023, Vol. 120 Issue 21, p1-7. 50p.
Publication Year :
2023

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. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
00278424
Volume :
120
Issue :
21
Database :
Academic Search Index
Journal :
Proceedings of the National Academy of Sciences of the United States of America
Publication Type :
Academic Journal
Accession number :
174701455
Full Text :
https://doi.org/10.1073/pnas.2220315120