Yu Zhichao, Xu Zhenjin, Zeng Ruijin, Xu Man, Zou Minglang, Huang Da, Weng Zuquan, Tang Dianping
Key Laboratory for Analytical Science of Food Safety and Biology (MOE & Fujian Province), Department of Chemistry, Fuzhou University, Fuzhou, 350108, China.
College of Biological Science and Engineering, Fuzhou University, Fuzhou, 350108, China.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202420200. doi: 10.1002/anie.202420200. Epub 2024 Nov 25.
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 14.903×10 min, which was 18.7 times higher than that of the Pt particles in monodisperse state in ZIF-8 (0.793×10 min). 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.
微生物抗生素耐药性威胁的不断升级加剧了全球细菌感染危机。纳米酶有望提供巧妙的解决方案。在此,我们报道了一种具有精细调节的金属有机框架(ZIF-8)通道结构的铂纳米簇的均相催化结构,用于治疗感染伤口。催化位点归一化显示,具有精细调节的孔修饰结构的铂聚集体结构的活性位点催化能力为14.903×10 min,比ZIF-8中处于单分散状态的铂颗粒(0.793×10 min)高18.7倍。原位测试表明,纳米酶界面处过氧化氢从均裂变为异裂的变化是纳米酶活性提高的关键原因之一。反应界面的密度泛函理论和动力学模拟共同确定了催化中心和底物通道的作用。代谢组学分析表明,所开发的纳米酶与活性氧共同作用,可有效阻断细菌内的能量代谢途径,导致细菌自发凋亡和破裂。这项开创性研究阐明了人工酶活性调控的新思路,为高效抗生素替代品的开发提供了新视角。
Angew Chem Int Ed Engl. 2025-2-10
Anal Chim Acta. 2024-6-22
ACS Appl Mater Interfaces. 2024-5-29
ACS Appl Mater Interfaces. 2020-4-15
Angew Chem Int Ed Engl. 2025-1-10
J Gastroenterol Hepatol. 2025-7
ACS Pharmacol Transl Sci. 2025-3-12