Sarker Prodip, Swindells Kathryn, Douglas C W Ian, MacNeil Sheila, Rimmer Stephen, Swanson Linda
Department of Chemistry, Brook Hill, University of Sheffield, Sheffield, South Yorkshire, UK S3 7HF.
Soft Matter. 2014 Aug 21;10(31):5824-35. doi: 10.1039/c4sm00056k. Epub 2014 Jun 30.
We describe a series of experiments designed to investigate the conformational transition that highly-branched polymers with ligands undergo when interacting with bacteria, a process that may provide a new sensing mechanism for bacterial detection. Fluorescent highly-branched poly(N-isopropyl acrylamide)s (HB-PNIPAM) were prepared by sequential self-condensing radical copolymerizations, using anthrylmethyl methacrylate (AMMA) and fluorescein-O-acrylate (FA) as fluorescent comonomers and 4-vinylbenzyl pyrrole carbodithioate as a branch forming monomer. Differences in reactivity necessitated to first copolymerize AMMA then react with FA in a separate sequential monomer feed step. Modifications of the chain ends produced vancomycin-functional derivatives (HB-PNIPAM-Van). The AMMA and FA labels allow probing of the conformational behaviour of the polymers in solution via Förster resonance energy transfer experiments. It was shown that interaction of this polymer's end groups with Staphylococcus aureus induced a macromolecular collapse. The data thus provide conclusive evidence for a conformational transition that is driven by binding to a bacterium.
我们描述了一系列实验,这些实验旨在研究带有配体的高度支化聚合物与细菌相互作用时所经历的构象转变,这一过程可能为细菌检测提供一种新的传感机制。通过顺序自缩合自由基共聚反应制备了荧光高度支化聚(N-异丙基丙烯酰胺)(HB-PNIPAM),使用甲基丙烯酸蒽甲酯(AMMA)和荧光素-O-丙烯酸酯(FA)作为荧光共聚单体,4-乙烯基苄基吡咯二硫代甲酸酯作为支化形成单体。由于反应活性的差异,需要先使AMMA共聚,然后在单独的顺序单体进料步骤中与FA反应。链端的修饰产生了万古霉素功能化衍生物(HB-PNIPAM-Van)。AMMA和FA标记允许通过Förster共振能量转移实验探测聚合物在溶液中的构象行为。结果表明,该聚合物端基与金黄色葡萄球菌的相互作用导致了大分子塌陷。因此,这些数据为因与细菌结合而驱动的构象转变提供了确凿证据。