School of Chemistry and Biosciences, University of Bradford, BD7 1DP, UK.
University of Sheffield, S3 7HF, UK.
J Mater Chem B. 2024 Nov 27;12(46):11996-12006. doi: 10.1039/d4tb01544d.
Highly branched poly(-isopropyl acrylamide) additives chain end functionalised with vancomycin have been designed to agglutinate and report on targetted Gram-positive strains of bacteria (). These branched systems selectively desolvate with temperature or binding interactions depending on their chain architecture. We have prepared samples with three different degrees of branching which have incorporated Nile red acrylate as a low concentration of co-monomer to report upon their solution properties. A linear analogue polymer functionalised with vancomycin along the chain instead of the termini is presented as a control which does not bind to targeted bacteria. These samples were analysed by diffusion NMR spectrometry (DOSY), calorimetry, fluorescence lifetime measurements, optical microscopy and scanning electron microscopy to gain a full understanding of their solution properties. The branched polymers are shown conclusively to have a core-shell structure, where the chain ends are expressed from the desolvated globule even above the lower critical solution temperature - as demonstrated by NMR measurements. The level of desolvation is critically dependent on the degree of branching, and as a result we have found intermediate structures provide optimal body temperature bacterial sensing as a consequence of the Nile red reporting dye.
已设计出具有万古霉素官能团的支化聚(异丙基丙烯酰胺)添加剂链端,以聚集和报告靶向的革兰氏阳性细菌菌株()。这些支化系统根据其链结构选择性地通过温度或结合相互作用去溶剂化。我们已经制备了三种不同支化度的样品,其中掺入尼罗红丙烯酰胺作为低浓度共聚单体来报告其溶液性质。沿链而不是末端官能化的线性类似物聚合物被用作对照,它不与靶向细菌结合。这些样品通过扩散 NMR 光谱(DOSY)、量热法、荧光寿命测量、光学显微镜和扫描电子显微镜进行分析,以全面了解其溶液性质。支化聚合物具有明显的核壳结构,其中链端从去溶剂化的球表达出来,甚至在低于下临界溶液温度之上 - 如 NMR 测量所示。去溶剂化的程度取决于支化度,因此我们发现中间结构由于尼罗红报告染料的存在提供了最佳的体温细菌传感。