摘要
      在本研究中，研究了引入的金属原子对金属-有机框架基纳米材料（MOFs）水解活性的空间位置效应。制备了在不同空间位置掺入单原子Cu的UiO型MOFs，发现它们对磷酸酯键的水解活性高度依赖于原子分散的Cu原子的位置。特别是，Cu原子与配体（UiO-67-CuN）的连接导致其水解活性的最显著增加，这可归因于MOFs的氧空位增加和Lewis酸度增加。结果，UiO-67-CuN有效地催化了作为DNA水解酶的DNA的切割，从而有效地抑制了ARGs的水平基因转移，消除了细菌对抗生素的耐药性。这项研究为合理设计基于MOF的高性能DNA水解酶和开发去除ARGs的新治疗策略开辟了新的前景。
Abstract
In this study, the spatial location effect of the incorporated metal atoms on the hydrolysis activity of metal organic framework-based nanomaterials (MOFs) was investigated. UiO-type MOFs incorporated with single-atom Cu at different spatial positions were prepared and their hydrolysis activity towards phosphoester bonds was found to be highly depended on the location of the atomically dispersed Cu atoms. Especially, the attachment of Cu atoms to ligand (UiO-67-CuN) resulted in the most significant increase of their hydrolysis activity, which can be attributed to the elevated oxygen vacancies and increased Lewis acidity of MOFs. As a result, UiO-67-CuN efficiently catalyzed the cleavage of DNA acting as DNA hydrolases, thereby effectively inhibiting the horizontal gene transfer of ARGs and eliminating bacterial resistance to antibiotic. This study opens up new prospects for the rational design of high-performance MOF-based DNA hydrolases and developing new treatment strategies for the removal of ARGs.

https://www.sciencedirect.com/science/article/pii/S0926337322008724