链式转移
共聚物
高分子化学
聚合
甲基丙烯酸酯
化学
位阻效应
可逆加成-断裂链转移聚合
两亲性
材料科学
自由基聚合
有机化学
聚合物
作者
Lei lei,Naganatha Patil,A. Arnoux,Clémence Le Cœur,Yoann de Rancourt de Mimérand,Daniel Grande,Benjamin Le Droumaguet,Xiaoshuang Feng,Yves Gnanou,Benoît Couturaud
出处
期刊:Macromolecules
[American Chemical Society]
日期:2024-11-12
卷期号:57 (22): 10513-10521
标识
DOI:10.1021/acs.macromol.4c01863
摘要
Semidegradable nanoparticles were synthesized in aqueous medium by photoinitiated polymerization-induced self-assembly, using a cleavable hydrophilic copolymer as a steric stabilizer that also served as a macromolecular chain transfer agent (mCTA) for the reversible addition–fragmentation chain transfer (RAFT) polymerization of 2-hydroxypropyl methacrylate (HPMA). This mCTA was obtained by modification of a pH-sensitive poly[(ethylene carbonate)-co-(ethylene oxide)] (PECEO) random copolymer that was end-fitted with a trithiocarbonate moiety. By adjusting the degree of polymerization of HPMA through RAFT, we achieved the synthesis of a series of amphiphilic block copolymers that self-assembled in various morphologies, including spheres, worms, and vesicles. Through characterization by 1H nuclear magnetic resonance, size exclusion chromatography, and transmission electron microscopy, it could be demonstrated that the carbonate linkages of their hydrophilic block and of their steric stabilizer undergo hydrolysis under alkaline conditions. The length of the PHPMA block and the balance between the hydrophilic and hydrophobic blocks are two parameters that have a significant impact on the self-assembly of these particles; a transition from steric to electrostatic stabilization of these nanoparticles could be witnessed during degradation for short PHPMA blocks. In summary, pH-sensitive nanoparticles sterically stabilized by degradable poly(ether-co-ether carbonate) copolymers gave rise under basic conditions to nanoparticles stabilized by electrostatic interaction.
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