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使用嵌入透明聚甲基丙烯酸羟乙酯水凝胶中的六核钼配合物对生物膜进行光动力灭活

Photodynamic Inactivation of Biofilms Using a Hexanuclear Molybdenum Complex Embedded in Transparent polyHEMA Hydrogels.

作者信息

López-López Noelia, Muñoz Resta Ignacio, de Llanos Rosa, Miravet Juan F, Mikhaylov Maxim, Sokolov Maxim N, Ballesta Sofía, García-Luque Isabel, Galindo Francisco

机构信息

Departamento de Química Inórganica y Orgánica, Universitat Jaume I, Av. Sos Baynat s/n, 12071 Castellón, Spain.

Unidad Predepartamental de Medicina, Universitat Jaume I, Av. Sos Baynat s/n, 12071 Castellón, Spain.

出版信息

ACS Biomater Sci Eng. 2020 Dec 14;6(12):6995-7003. doi: 10.1021/acsbiomaterials.0c00992. Epub 2020 Nov 19.

Abstract

Three new photoactive polymeric materials embedding a hexanuclear molybdenum cluster (BuN)[MoI(CHCOO)] () have been synthesized and characterized by means of Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and emission spectroscopy. The materials are obtained in the format of transparent and thin sheets, and the formulations used to synthesize them are comprised of 2-hydroxyethyl methacrylate (HEMA), as a polymerizable monomer, and ethylene glycol dimethacrylate (EGDMA) or poly(ethylene glycol)dimethacrylate (PEGDMA), as cross-linkers. All the polymeric hydrogels generate singlet oxygen (O) upon irradiation with visible light (400-700 nm), as demonstrated by the reactivity toward two chemical traps of this reactive species (9,10-dimethylanthracene and 1,5-dihydroxynaphthalene). Some differences have been detected between the photoactive materials, probably attributable to variations in the permeability to solvent and oxygen. Notably, one of the materials resisted up to 10 cycles of photocatalytic oxygenation reactions of 1,5-dihydroxynaphthalene. All three of the polyHEMA hydrogels doped with are efficient against biofilms when irradiated with blue light (460 nm). The material made with the composition of 90% HEMA and 10% PEGDMA () is especially easy to handle, because of its flexibility, and it achieves a notable level of bacterial population reduction (3.0 log CFU/cm). The embedding of in cross-linked polyHEMA sheets affords a protective environment to the photosensitizer against aqueous degradation while preserving the photochemical and photobactericidal activity.

摘要

三种嵌入六核钼簇(BuN)[MoI(CHCOO)]()的新型光活性聚合物材料已通过傅里叶变换红外光谱(FTIR)、热重分析(TGA)和发射光谱进行了合成与表征。这些材料以透明薄片的形式获得,用于合成它们的配方由作为可聚合单体的甲基丙烯酸2 - 羟乙酯(HEMA)以及作为交联剂的乙二醇二甲基丙烯酸酯(EGDMA)或聚乙二醇二甲基丙烯酸酯(PEGDMA)组成。所有聚合物水凝胶在可见光(400 - 700 nm)照射下都会产生单线态氧(O),这通过其对该活性物种的两种化学捕获剂(9,10 - 二甲基蒽和1,5 - 二羟基萘)的反应性得到了证明。在光活性材料之间检测到了一些差异,这可能归因于对溶剂和氧气的渗透性变化。值得注意的是,其中一种材料在1,5 - 二羟基萘的光催化氧化反应中能耐受多达10个循环。所有三种掺杂的聚HEMA水凝胶在蓝光(460 nm)照射下对生物膜都有高效的抗菌效果。由90% HEMA和10% PEGDMA()组成的材料因其柔韧性特别易于处理,并且能显著降低细菌数量(3.0 log CFU/cm)。将嵌入交联聚HEMA片中为光敏剂提供了一个免受水降解的保护环境,同时保留了光化学和光杀菌活性。

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