4.8 Article

Modulating the local coordination environment of cobalt single-atomic nanozymes for enhanced catalytic therapy against bacteria

Journal

ACTA BIOMATERIALIA
Volume 164, Issue -, Pages 563-576

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.actbio.2023.03.040

Keywords

Single-atomic nanozymes; Adjusting the coordination number; Catalytic antibacterial therapy; Wound disinfection

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Single-atomic nanozymes characterized by atomically dispersed single metal atoms have shown satisfactory catalytic activity and superior selectivity compared to their nanoscale counterparts, contributing to breakthroughs in biomedicine. Adjusting the coordination number of the metal atoms can improve their catalytic performance. In this study, atomically dispersed Co nanozymes with different nitrogen coordination numbers were synthesized, and it was found that Co nanozymes with a coordination number of 2 had the highest catalytic activity and antibacterial effect. This research provides proof of concept for enhancing single-atomic catalytic therapy by regulating the coordination number for various biomedical applications.
Single-atomic nanozymes (SANZs) characterized by atomically dispersed single metal atoms have recently contributed to breakthroughs in biomedicine due to their satisfactory catalytic activity and superior se-lectivity compared to their nanoscale counterparts. The catalytic performance of SANZs can be improved by modulating their coordination structure. Therefore, adjusting the coordination number of the metal atoms in the active center is a potential method for enhancing the catalytic therapy effect. In this study, we synthesized various atomically dispersed Co nanozymes with different nitrogen coordination numbers for peroxidase (POD)-mimicking single-atomic catalytic antibacterial therapy. Among the polyvinylpyrroli-done modified single-atomic Co nanozymes with nitrogen coordination numbers of 3 (PSACNZs-N3-C) and 4 (PSACNZs-N4-C), single-atomic Co nanozymes with a coordination number of 2 (PSACNZs-N2-C) had the highest POD-like catalytic activity. Kinetic assays and Density functional theory (DFT) calculations indi-cated that reducing the coordination number can lower the reaction energy barrier of single-atomic Co nanozymes (PSACNZs-Nx-C), thereby increasing their catalytic performance. In vitro and in vivo antibacte-rial assays demonstrated that PSACNZs-N2-C had the best antibacterial effect. This study provides proof of concept for enhancing single-atomic catalytic therapy by regulating the coordination number for various biomedical applications, such as tumor therapy and wound disinfection. Statement of significance The use of nanozymes that contain single-atomic catalytic sites has been shown to effectively promote the healing of bacteria-infected wounds by exhibiting peroxidase-like activity. The homogeneous coor-dination environment of the catalytic site has been associated with high antimicrobial activity, which provides insight into designing new active structures and understanding their mechanisms of action. In this study, we designed a series of cobalt single-atomic nanozymes (PSACNZs-Nx-C) with different coor-dination environments by shearing the Co-N bond and modifying polyvinylpyrrolidone (PVP). The synthe-sized PSACNZs-Nx-C demonstrated enhanced antibacterial activity against both Gram-positive and Gram-negative bacterial strains, and showed good biocompatibility in both in vivo and in vitro experiments. & COPY; 2023 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

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