Effect of Composition on the Thermo-Induced Aggregation of Poloxamer-Analogue Triblock Terpolymers

IF 5.2 1区化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2025-02-26 DOI:10.1021/acs.macromol.4c02217

Shaobai Wang, Alberto Alvarez-Fernandez, Xu Liu, Sofia Miron-Barroso, Kelvin Wong, Stefan Guldin, Theoni K. Georgiou

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Abstract

Thermoresponsive polymers hold great promise for biomedical applications due to their thermo-induced phase transitions. However, challenges including controlling transition temperatures, aggregate behavior, or complex synthesis, have limited their broader use. In this study, six ABC triblock terpolymers were synthesized via group transfer polymerization, targeting a molar mass of 8000 g/mol with varying compositions. The terpolymers consist of hydrophilic oligo(ethylene glycol) methyl ether methacrylate (average molar mass = 300 g/mol, OEGMA300), hydrophobic di(propylene glycol) methyl ether methacrylate (diPGMA), and less-hydrophilic di(ethylene glycol) methyl ether methacrylate (DEGMA). Systematic characterizations of properties related to thermo-induced aggregation, including cloud point temperature, aggregate morphology, and chain immobilization, identified a unique dual-stage phase transition in the terpolymer containing 45 wt % OEGMA300, 35 wt % diPGMA, and 20 wt % DEGMA. Instead of directly agglomerating into globular aggregates, this terpolymer transitioned from spherical micelles to vesicular species, offering valuable insights for the design of controllable and responsive polymer systems.

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成分对聚氧乙烯-类似物三嵌段三元共聚物热诱导聚合的影响

热响应聚合物由于其热诱导相变而在生物医学应用中具有很大的前景。然而，包括控制转变温度、聚合行为或复杂合成在内的挑战限制了它们的广泛应用。本研究通过基团转移聚合合成了6种ABC三嵌段三元共聚物，其组成不同，摩尔质量为8000g /mol。三元共聚物由亲水性低聚（乙二醇）甲基醚甲基丙烯酸甲酯（平均摩尔质量= 300 g/mol, OEGMA300）、疏水性二（丙二醇）甲基醚甲基丙烯酸甲酯（diPGMA）和亲水性较低的二（乙二醇）甲基醚甲基丙烯酸甲酯（DEGMA）组成。系统表征了与热诱导聚集相关的性质，包括云点温度、聚集形态和链固定，确定了含有45 wt % OEGMA300、35 wt % diPGMA和20 wt % DEGMA的三元聚合物的独特的双阶段相变。这种三元共聚物不是直接聚集成球状聚集体，而是从球形胶束转变为囊状物质，这为设计可控和响应性聚合物体系提供了有价值的见解。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.