Affiliation:
1. Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of Chemistry Tianjin University Tianjin 300072 China
2. The Province and Ministry Co‐Sponsored Collaborative Innovation Center for Medical Epigenetics Tianjin Key Laboratory of Technologies Enabling Development of Clinical Therapeutics and Diagnostics School of Pharmacy Tianjin Medical University Tianjin 300070 China
Abstract
AbstractSingle‐atom nanozymes (SAzymes) hold great promise in tumor therapy due to their maximized atomic utilization and well‐defined electronic structures. However, they still face challenges of activity, specificity, and targeting that impede therapeutic efficacy. Herein, a practical strategy is reported to construct asymmetric N, S‐coordinated Fe SAzymes (Fe‐S/N‐C). Benefiting from the regulatory influence of S atoms on the disruption of local charge symmetry of center Fe atoms, the Fe‐S/N‐C SAzymes exhibit significantly enhanced peroxidase (POD)‐ and glutathione oxidase (GSHOx)‐like activities, with catalytic efficiencies being 6.33 and 47.88 times higher than their symmetric Fe‐N4 counterparts, respectively. Theoretical calculations demonstrate that the asymmetric atomic interface configuration increases electron localization around center Fe sites, thus facilitating the adsorption and activation of H2O2 and O2. By camouflaging with macrophage membranes, the tumor‐targeting nanocatalytic agents (M@Fe‐S/N‐C) trigger enhanced self‐cascade catalysis in the tumor microenvironment for ferroptosis‐based tumor‐specific therapy. These results open up a promising avenue for addressing the limitations associated with current SAzymes‐based tumor therapies.
Funder
National Natural Science Foundation of China
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials