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Stimuli-responsive microgels with cationic moieties: characterization and interaction with E. coli cells
Soft Matter ( IF 2.9 ) Pub Date : 2021-09-14 , DOI: 10.1039/d1sm01007g
Larissa Hussmann 1, 2 , Thomke Belthle 1, 2 , Dan E Demco 1, 3 , Radu Fechete 3 , Andrij Pich 1, 2, 4
Affiliation  

Stimuli-responsive microgel copolymer networks with ionizable functional groups have important applications for encapsulation of drugs, peptides, enzymes, proteins, or cells. Rational design of such networks can be based on characterization of stimuli-induced volume phase transition and spatial distribution of neutral and charged monomer units in crosslinked polymer chains. In this work we successfully synthesized poly(N-vinylcaprolactam-co-1-vinyl-3-methylimidazolium) (poly(VCL-VIM+)) microgels carrying permanent positive charges and demonstrate that 1H high-resolution NMR spectroscopy in combination with transverse (T2) magnetization relaxometry allows investigating separately the behavior of each functional group in the microgel network. The information about comonomer transition temperatures, width of transition, and change in transition entropy were reported and correlated with the concentration of charged functional groups and resulting electrophoretic mobility. A two-state approach was used to describe the temperature-induced volume phase transition separately for neutral and charged polymer segments. The core–corona architecture specific to each functional group was detected revealing that the charged methylated vinylimidazolium groups (VIM+) are concentrated mainly in the corona of the microgel. These biocompatible PVCL-based microgels functionalized with permanent positive charges are shown to serve as an antibacterial system against Gram-negative E. coli strains, due to the positive charge of the incorporated VIM+ comonomer in the polymer network.

中文翻译:

具有阳离子部分的刺激响应微凝胶:表征和与大肠杆菌细胞的相互作用

具有可电离官能团的刺激响应微凝胶共聚物网络在药物、肽、酶、蛋白质或细胞的封装方面具有重要应用。这种网络的合理设计可以基于刺激诱导的体积相变和交联聚合物链中中性和带电单体单元的空间分布的表征。在这项工作中,我们成功地合成了聚(Ñ -vinylcaprolactam--1-乙烯基-3-甲基咪唑鎓)(聚(VCL-VIM +))微凝胶携带永久正电荷,并证明1个与横向联合H高解析度NMR光谱(Ť 2) 磁化弛豫允许分别研究微凝胶网络中每个官能团的行为。报告了关于共聚单体转变温度、转变宽度和转变熵变化的信息,并与带电官能团的浓度和由此产生的电泳迁移率相关联。一种二态方法用于分别描述中性和带电聚合物链段的温度诱导体积相变。检测到每个官能团特有的核-电晕结构,表明带电的甲基化乙烯基咪唑鎓基团(VIM +) 主要集中在微凝胶的电晕中。由于聚合物网络中掺入的 VIM +共聚单体的正电荷,这些具有永久性正电荷功能化的基于生物相容性 PVCL 的微凝胶被证明可用作对抗革兰氏阴性大肠杆菌菌株的抗菌系统。
更新日期:2021-09-14
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