A Bioinspired Five-Coordinated Single-Atom Iron Nanozyme for Tumor Catalytic Therapy,Advanced Materials

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A Bioinspired Five-Coordinated Single-Atom Iron Nanozyme for Tumor Catalytic Therapy
Advanced Materials ( IF 27.4 ) Pub Date : 2022-01-31 , DOI: 10.1002/adma.202107088
Bolong Xu ₁ , Shanshan Li ₁ , Lirong Zheng ₂ , Yunhang Liu ₁ , Along Han ₁ , Jin Zhang ₁ , Zhijun Huang ₃ , Haijiao Xie ₄ , Kelong Fan ₅ , Lizeng Gao ₅ , Huiyu Liu ₁

Affiliation

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 × 10⁵ 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.

中文翻译：

一种用于肿瘤催化治疗的仿生五配位单原子铁纳米酶

单原子纳米酶（SAzymes）代表了生物医学领域的一个新的研究前沿。具有明确定义的电子和几何结构的 SAzymes 的合理设计和可控合成对于最大限度地提高其酶样催化活性和治疗效果至关重要，但仍然具有挑战性。_{在这里，报道了一种三聚氰胺介导的热解活化策略，用于可控制造含有五配位结构 (FeN 5} )的铁基 SAzyme ，通过透射电子显微镜成像和 X 射线吸收精细结构分析确定。由于优化的配位结构， FeN ₅ SAzyme 表现出优异的类过氧化物酶活性，以及 FeN _{5中 Fe 物种的相应催化效率}稳态动力学测定表明，SAzyme 分别是传统 FeN ₄ SAzyme 和 Fe ₃ O ₄纳米酶的 7.64 和 3.45 × 10 ⁵倍。此外，催化机理由实验结果和密度泛函理论研究共同揭示。由于在肿瘤微环境下具有优异的过氧化物酶样活性，所合成的 FeN ₅ SAzyme 在体外和体内均表现出显着增强的抗肿瘤作用。

更新日期：2022-01-31

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