Beijing Advanced Innovation Center for Soft Matter Science and Engineering, State Key Laboratory of Organic-Inorganic Composites, Bionanomaterials & Translational Engineering Laboratory, Beijing Key Laboratory of Bioprocess, Beijing Laboratory of Biomedical Materials, Beijing University of Chemical Technology, Beijing, 100029, China.
Laboratory of Theoretical and Computational Nanoscience, CAS Key Laboratory of Nanosystem and Hierarchial Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, 100190, China.
Angew Chem Int Ed Engl. 2019 Apr 1;58(15):4911-4916. doi: 10.1002/anie.201813994. Epub 2019 Mar 5.
Single-atom catalysts (SACs), as homogeneous catalysts, have been widely explored for chemical catalysis. However, few studies focus on the applications of SACs in enzymatic catalysis. Herein, we report that a zinc-based zeolitic-imidazolate-framework (ZIF-8)-derived carbon nanomaterial containing atomically dispersed zinc atoms can serve as a highly efficient single-atom peroxidase mimic. To reveal its structure-activity relationship, the structural evolution of the single-atom nanozyme (SAzyme) was systematically investigated. Furthermore, the coordinatively unsaturated active zinc sites and catalytic mechanism of the SAzyme are disclosed using density functional theory (DFT) calculations. The SAzyme, with high therapeutic effect and biosafety, shows great promises for wound antibacterial applications.
单原子催化剂(SACs)作为均相催化剂,在化学催化中得到了广泛的研究。然而,很少有研究关注 SACs 在酶催化中的应用。在此,我们报道了一种基于锌的沸石咪唑酯骨架(ZIF-8)衍生的含原子分散锌原子的碳纳米材料可用作高效的单原子过氧化物酶模拟物。为了揭示其结构-活性关系,系统地研究了单原子纳米酶(SAzyme)的结构演变。此外,使用密度泛函理论(DFT)计算揭示了 SAzyme 的配位不饱和活性锌位点和催化机制。具有高治疗效果和生物安全性的 SAzyme 显示出在伤口抗菌应用方面的巨大潜力。