Modulating Electron Transfer in Vanadium-Based Artificial Enzymes for Enhanced ROS-Catalysis and Disinfection
© 2022 Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 17 vom: 21. Apr., Seite e2108646 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2022
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article ROS-based biocatalysis antibacterial and wound healing artificial enzymes electron modulation inorganic nanomaterials Reactive Oxygen Species Vanadium 00J9J9XKDE |
Zusammenfassung: | © 2022 Wiley-VCH GmbH. Nanomaterials-based artificial enzymes (AEs) have flourished for more than a decade. However, it is still challenging to further enhance their biocatalytic performances due to the limited strategies to tune the electronic structures of active centers. Here, a new path is reported for the de novo design of the d electrons of active centers by modulating the electron transfer in vanadium-based AEs (VOx -AE) via a unique Zn-O-V bridge for efficient reactive oxygen species (ROS)-catalysis. Benefiting from the electron transfer from Zn to V, the V site in VOx -AE exhibits a lower valence state than that in V2 O5 , which results in charge-filled V-dyz orbital near the Fermi level to interfere with the formation of sigma bonds between the V- d z 2 and O-pz orbitals in H2 O2 . The VOx -AE exhibits a twofold Vmax and threefold turnover number than V2 O5 when catalyzing H2 O2 . Meanwhile, the VOx -AE shows enhanced catalytic eradication of drug-resistant bacteria and achieves comparable wound-treatment indexes to vancomycin. This modulating charge-filling of d electrons provides a new direction for the de novo design of nanomaterials-based AEs and deepens the understanding of ROS-catalysis |
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Beschreibung: | Date Completed 28.04.2022 Date Revised 28.04.2022 published: Print-Electronic Citation Status MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202108646 |