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一种用于对抗植入相关感染的金纳米团簇构建的混合金属金属有机网络薄膜。

A Gold Nanocluster Constructed Mixed-Metal Metal-Organic Network Film for Combating Implant-Associated Infections.

作者信息

Chu Guangyu, Zhang Chunlei, Liu Yifei, Cao Zanxia, Wang Lirui, Chen Yunfeng, Zhou Wenjie, Gao Guo, Wang Kan, Cui Daxiang

机构信息

Department of Orthopedic Surgery, Shanghai Jiao Tong University Affiliated Sixth People's Hospital, 600 Yishan Road, Shanghai, 200233, China.

Institute of Nano Biomedicine and Engineering, Shanghai Engineering Research Center for Intelligent Diagnosis and Treatment Instrument, Department of Instrument Science & Engineering, School of Electronic Information and Electrical Engineering Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.

出版信息

ACS Nano. 2020 Nov 24;14(11):15633-15645. doi: 10.1021/acsnano.0c06446. Epub 2020 Nov 9.

Abstract

The development of modular strategies for programming self-assembled supramolecular architectures with distinct structural and functional features is of immense scientific interest. We reported on the intrinsic antibacterial capability of anionic amphiphilic gold nanoclusters (GNCs) capped by -mercaptobenzoic acid, which was closely related to the protonation level of terminal carboxylate groups. By using of the metal-ligand coordination-driven and solvent evaporation-induced self-assembly, we constructed GNCs-based mixed-metal metal-organic network (MM-MON) films on titanium disks as antibacterial nanocoatings. Taking the reasonable utilization of tetravalent metal ions M (Ti, Zr, Hf; hard Lewis acid) and bactericidal divalent metal ions M (Cu, Zn; borderline acid) co-incorporated metal-carboxylate coordination bonds, the MM-MON films exhibited superior stability due to the robust M-O bonds and M releasing behavior resulting from the labile M-O coordinating. Together, the MM-MON films integrated the bacteria-responsive character of GNCs, exceptional chemical stability, and greatly enhanced antibacterial activity, ultimately killing adherent bacteria and initiating a self-defensive function. In a rat model for subcutaneous implant-associated infection, the MM-MON nanocoating showed an approximately 2 and 1 log lower multidrug-resistant implant and tissue colonization, respectively. The generalizable modular strategy of the GNC-metal networks is amenable to facilitate the functionalization of metal surfaces for combating implant-associated infections.

摘要

开发用于编程具有独特结构和功能特征的自组装超分子结构的模块化策略具有巨大的科学意义。我们报道了由巯基苯甲酸封端的阴离子两亲性金纳米团簇(GNCs)的固有抗菌能力,这与末端羧酸盐基团的质子化水平密切相关。通过利用金属-配体配位驱动和溶剂蒸发诱导的自组装,我们在钛盘上构建了基于GNCs的混合金属金属有机网络(MM-MON)薄膜作为抗菌纳米涂层。合理利用四价金属离子M(Ti, Zr, Hf;硬路易斯酸)和杀菌二价金属离子M(Cu, Zn;边界酸)共掺入的金属-羧酸盐配位键,MM-MON薄膜由于坚固的M-O键和不稳定的M-O配位导致的M释放行为而表现出优异的稳定性。总之,MM-MON薄膜整合了GNCs的细菌响应特性、出色 的化学稳定性和大大增强的抗菌活性,最终杀死粘附的细菌并启动自我防御功能。在皮下植入相关感染的大鼠模型中,MM-MON纳米涂层显示多药耐药植入物和组织定植分别降低了约2个对数和1个对数。GNC-金属网络的可推广模块化策略有利于促进金属表面的功能化,以对抗植入相关感染。

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