High Fe‑Loading Single‑Atom Catalyst Boosts ROS Production by Density Effect for Efficient Antibacterial Therapy  

作　　者：Si Chen Fang Huang Lijie Mao Zhimin Zhang Han Lin Qixin Yan Xiangyu Lu Jianlin Shi 

机构地区：[1]Department of Cardiology,Shanghai Tenth People’s Hospital,School of Medicine,Tongji University,Shanghai 200092,People’s Republic of China [2]Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 200050,People’s Republic of China [3]Shanghai Frontiers Science Center of Nanocatalytic Medicine,School of Medicine,Tongji University,Shanghai 200092,People’s Republic of China

出　　处：《Nano-Micro Letters》2025年第2期187-203,共17页纳微快报（英文版）

基　　金：supported by the National Key Research and Development Program of China(Grant No.2022YFB3804500);the National Natural Science Foundation of China(Grant No.52202352,22335006);the Shanghai Municipal Health Commission(Grant No.20224Y0010);the CAMS Innovation Fund for Medical Sciences(Grant No.2021-I2M-5-012);the Basic Research Program of Shanghai Municipal Government(Grant No.21JC1406000);the Fundamental Research Funds for the Central Universities(Grant No.22120230237,2023-3-YB-11,22120220618);the Basic Research Program of Shanghai Municipal Government(23DX1900200).

摘　　要：The current single-atom catalysts(SACs)for medicine still suffer from the limited active site density.Here,we develop a synthetic method capable of increasing both the metal loading and mass-specific activity of SACs by exchanging zinc with iron.The constructed iron SACs(h^(3)-FNC)with a high metal loading of 6.27 wt%and an optimized adjacent Fe distance of~4 A exhibit excellent oxidase-like catalytic performance without significant activity decay after being stored for six months and promising antibacterial effects.Attractively,a“density effect”has been found at a high-enough metal doping amount,at which individual active sites become close enough to interact with each other and alter the electronic structure,resulting in significantly boosted intrinsic activity of single-atomic iron sites in h^(3)-FNCs by 2.3 times compared to low-and medium-loading SACs.Consequently,the overall catalytic activity of h^(3)-FNC is highly improved,with mass activity and metal mass-specific activity that are,respectively,66 and 315 times higher than those of commercial Pt/C.In addition,h^(3)-FNCs demonstrate efficiently enhanced capability in catalyzing oxygen reduction into superoxide anion(O_(2)·^(−))and glutathione(GSH)depletion.Both in vitro and in vivo assays demonstrate the superior antibacterial efficacy of h^(3)-FNCs in promoting wound healing.This work presents an intriguing activity-enhancement effect in catalysts and exhibits impressive therapeutic efficacy in combating bacterial infections.

关 键 词：Nanocatalytic medicine Single-atom catalysts Reactive oxygen species(ROS) High metal loading Oxidase catalysis 

分 类 号：R914[医药卫生—药物化学] O643.36[医药卫生—药学]