Engineering Atomically Dispersed Cu–N1S2 Sites via Chemical Vapor Deposition to Boost Enzyme‐Like Activity for Efficient Tumor Therapy
-
Published:2023-12-24
Issue:
Volume:
Page:
-
ISSN:0935-9648
-
Container-title:Advanced Materials
-
language:en
-
Short-container-title:Advanced Materials
Author:
Xu Bolong1ORCID,
Li Shanshan1,
Han Along1,
Zhou You2,
Sun Mengxue1,
Yang Haokun1,
Zheng Lirong3,
Shi Rui2,
Liu Huiyu1ORCID
Affiliation:
1. Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic‐Inorganic Composites Bionanomaterials and Translational Engineering Laboratory Beijing Key Laboratory of Bioprocess Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology Beijing 100029 China
2. National Center for Orthopaedics Beijing Research Institute of Traumatology and Orthopaedics Beijing Jishuitan Hospital Beijing 100035 China
3. Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China
Abstract
AbstractSingle‐atom nanozymes (SAzymes), with well‐defined and uniform atomic structures, are an emerging type of natural enzyme mimics. Currently, it is important but challenging to rationally design high‐performance SAzymes and deeply reveal the interaction mechanism between SAzymes and substrate molecules. Herein, this work reports the controllable fabrication of a unique Cu−N1S2‐centred SAzyme (Cu‐N/S‐C) via a chemical vapor deposition‐based sulfur‐engineering strategy. Benefiting from the optimized geometric and electronic structures of single‐atom sites, Cu‐N/S‐C SAzyme shows boosted enzyme‐like activity, especially in catalase‐like activity, with a 13.8‐fold increase in the affinity to hydrogen peroxide (H2O2) substrate and a 65.2‐fold increase in the catalytic efficiency when compared to Cu‐N‐C SAzyme with Cu−N3 sites. Further theoretical studies reveal that the increased electron density around single‐atom Cu is achieved through electron redistribution, and the efficient charge transfer between Cu‐N/S‐C and H2O2 is demonstrated to be more beneficial for the adsorption and activation of H2O2. The as‐designed Cu‐N/S‐C SAzyme possesses an excellent antitumor effect through the synergy of catalytic therapy and oxygen‐dependent phototherapy. This study provides a strategy for the rational design of SAzymes, and the proposed electron redistribution and charge transfer mechanism will help to understand the coordination environment effect of single‐atom metal sites on H2O2‐mediated enzyme‐like catalytic processes.
Funder
National Key Research and Development Program of China
National Natural Science Foundation of China
Fundamental Research Funds for the Central Universities
China Postdoctoral Science Foundation
Beijing Municipal Health Commission
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science