School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Macromol Rapid Commun. 2021 Apr;42(8):e2000652. doi: 10.1002/marc.202000652. Epub 2020 Dec 28.
A modular strategy for the synthesis of dendron-linear polymer hybrids comprised of a flexible polydimethylsiloxane (PDMS) midblock with cationic 2,2-bis(hydroxymethyl)propionic acid (bis-MPA) dendron end groups is developed. The invention of a scalable methodology to access quaternary ammonium carboxylate building blocks and their direct use in esterification chemistry enables rapid access to cationic bis-MPA dendrons. The convergent click coupling of highly charged dendrons to hydrophobic PDMS chain-ends gives a 12-membered family of hybrids that are comprised of different dendron generations (G1-3) and quaternary ammonium alkyl chain lengths (C , C , C , C ). This provides a library of materials with variable hydrophobicity, charge density, and chain-end valency. The physical behavior of the dendron-linear PDMS hybrid copolymers significantly changes after introduction of the cationic dendron end-groups and leads to soft-solid materials as a result of inhibited chain mobility. These PDMS-dendron hybrids are expected to behave as surface-active antimicrobial additives in bulk cross-linked silicone systems.
开发了一种由柔性聚二甲基硅氧烷(PDMS)中嵌段和阳离子 2,2-双(羟甲基)丙酸(bis-MPA)树枝状端基组成的树枝状-线性聚合物杂化物的模块化合成策略。发明了一种可扩展的方法来获得季铵羧酸酯砌块,并直接将其用于酯化反应中,从而可以快速获得阳离子 bis-MPA 树枝状分子。带高电荷的树枝状分子与疏水性 PDMS 链端的收敛点击偶联,得到由不同树枝代(G1-3)和季铵烷基链长(C 、C 、C 、C )组成的 12 种杂化物家族。这提供了一系列具有可变疏水性、电荷密度和链端价态的材料。引入阳离子树枝状端基后,树枝状-线性 PDMS 杂化物共聚物的物理行为发生显著变化,导致链迁移受到抑制,从而形成软固态材料。这些 PDMS-树枝状杂化物有望在交联硅酮体系中作为具有表面活性的抗菌添加剂。