期刊
ADVANCED MATERIALS
卷 34, 期 15, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202107088
关键词
bioinspired design; peroxidase-like activity; single-atom nanozymes; tumor catalytic therapy
类别
资金
- National Natural Science Foundation of China [21822802, 51772018, 22061130205]
- National Key Research and Development Program of China [2016YFA0201500]
- Fundamental Research Funds for the Central Universities [XK1802-8, buctrc201915]
Single-atom nanozymes are a new research frontier in the biomedical fields. A melamine-mediated pyrolysis activation strategy has been used to controllably fabricate iron-based SAzymes with a five-coordinated structure (FeN5). The FeN5 SAzyme shows excellent peroxidase-like activity and significantly enhanced antitumor effect in vitro and in vivo.
Single-atom nanozymes (SAzymes) represent a new research frontier in the biomedical fields. The rational design and controllable synthesis of SAzymes with well-defined electronic and geometric structures are essential for maximizing their enzyme-like catalytic activity and therapeutic efficacy but remain challenging. Here, a melamine-mediated pyrolysis activation strategy is reported for the controllable fabrication of iron-based SAzyme containing five-coordinated structure (FeN5), identified by transmission electron microscopy imaging and X-ray absorption fine structure analyses. The FeN5 SAzyme exhibits superior peroxidase-like activity owing to the optimized coordination structure, and the corresponding catalytic efficiency of Fe-species in the FeN5 SAzyme is 7.64 and 3.45 x 10(5) times higher than those in traditional FeN4 SAzyme and Fe3O4 nanozyme, respectively, demonstrated by steady-state kinetic assay. In addition, the catalytic mechanism is jointly disclosed by experimental results and density functional theory studies. The as-synthesized FeN5 SAzyme demonstrates significantly enhanced antitumor effect in vitro and in vivo due to the excellent peroxidase-like activity under tumor microenvironment.
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