基于金属有机框架的定制纳米酶用于增强类酶催化。

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhichao Yu, Zhenjin Xu, Ruijin Zeng, Man Xu, Minglang Zou, Da Huang, Zuquan Weng, Dianping Tang
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引用次数: 0

摘要

微生物抗生素耐药性的威胁不断升级,加剧了全球细菌感染的危机。纳米酶有望提供巧妙的解决方案。在此,我们报告了一种具有微调金属有机框架(ZIF-8)通道结构的铂纳米团簇的均相催化结构,用于治疗感染伤口。催化位点归一化显示,具有微调孔道修饰结构的铂聚集体结构的活性位点的催化能力为 14.903 ×105 min-1,是 ZIF-8 中单分散状态铂颗粒(0.793 ×105 min-1)的 18.7 倍。原位测试表明,纳米酶界面上的过氧化氢从同leavage 到异leavage 的变化是纳米酶活性提高的关键原因之一。反应界面的密度函数理论和动力学模拟共同确定了催化中心和底物通道的共同作用。代谢组学分析表明,开发的纳米酶与活性氧共同作用,能有效阻断细菌体内的能量代谢途径,导致细菌自发凋亡和细菌破裂。这项开创性的研究阐明了人工酶活性调控的新思路,为开发高效抗生素替代品提供了新的视角。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Tailored Metal-Organic Framework-Based Nanozymes for Enhanced Enzyme-Like Catalysis.

The global crisis of bacterial infections is exacerbated by the escalating threat of microbial antibiotic resistance. Nanozymes promise to provide ingenious solutions. Here, we reported a homogeneous catalytic structure of Pt nanoclusters with finely tuned metal-organic framework (ZIF-8) channel structures for the treatment of infected wounds. Catalytic site normalization showed that the active site of the Pt aggregates structure with fine-tuned pore modifications structure had a catalytic capacity of 14.903×105 min-1, which was 18.7 times higher than that of the Pt particles in monodisperse state in ZIF-8 (0.793×105 min-1). In situ tests revealed that the change from homocleavage to heterocleavage of hydrogen peroxide at the interface of the nanozyme was one of the key reasons for the improvement of nanozyme activity. Density-functional theory and kinetic simulations of the reaction interface jointly determine the role of the catalytic center and the substrate channel together. Metabolomics analysis showed that the developed nanozyme, working in conjunction with reactive oxygen species, could effectively block energy metabolic pathways within bacteria, leading to spontaneous apoptosis and bacterial rupture. This pioneering study elucidates new ideas for the regulation of artificial enzyme activity and provides new perspectives for the development of efficient antibiotic substitutes.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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