1. Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis.
- Author
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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, and Chengzhou Zhu
- Subjects
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ORGANOPHOSPHORUS pesticides , *CATALYSIS , *CHARGE exchange , *METAL-organic frameworks , *SYNTHETIC enzymes , *PRODUCT recovery - 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]
- Published
- 2023
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