Photoexcited Ru single-atomic sites for efficient biomimetic redox catalysis

• DOI: 10.1073/pnas.2220315120
• Publication Date: 2023-05-15T19:15:35Z
• Authors: Weiqing Xu; Hong Zhong; Yu Wu; Ying Qin; Lei Jiao; Meng Sha; Rina Su; Yinjun Tang; Lirong Zheng; Liuyong Hu; Shipeng Zhang; Scott P. Beckman; Wenling Gu; Yong Yang; Shaojun Guo; Chengzhou Zhu
• Keywords: Organophosphorus Compounds; Biomimetics; Physical Sciences; Hydrogen Peroxide; Pesticides; Oxidation-Reduction; 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 photoelectron transfers natural photoenzymes, we herein report a photonanozyme single-atom Ru anchored on metal-organic frameworks (UiO-67-Ru) for achieving photoenhanced peroxidase (POD)-like activity. We demonstrate that atomically dispersed sites can realize high photoelectric conversion efficiency, superior POD-like (7.0-fold photoactivity enhancement relative UiO-67), and good specificity. Both situ experiments theoretical calculations reveal photoelectrons follow cofactor-mediated ET process enzymes promote production active intermediates release products, demonstrating more favorable thermodynamics kinetics H2O2 reduction. Taking advantage unique interaction Zr-O-P bond, establish UiO-67-Ru-based immunoassay platform detection organophosphorus pesticides.