Tuning Micellization and Dissociation Transitions of Thermo- and pH-Sensitive Poly(ethylene oxide)-b-poly(methoxydi(ethylene glycol) methacrylate-co-methacrylic acid) in Aqueous Solution by Combining Temperature and pH Triggers

环氧乙烷 共聚物 高分子化学 甲基丙烯酸酯 化学 乙二醇 水溶液 胶束 甲基丙烯酸 低临界溶液温度 离解(化学) 浊点 聚合 临界胶束浓度 聚合物 有机化学
作者
Xueguang Jiang,Bin Zhao
出处
期刊:Macromolecules [American Chemical Society]
卷期号:41 (23): 9366-9375 被引量:79
标识
DOI:10.1021/ma8018238
摘要

We report in this article on the active control of multiple micellization and dissociation transitions of thermo- and pH-sensitive water-soluble block copolymers, poly(ethylene oxide)-b-poly(methoxydi(ethylene glycol) methacrylate-co-methacrylic acid) (PEO-b-P(DEGMMA-co-MAA)), in aqueous solutions by combining temperature and pH triggers. Two block copolymers and one random copolymer P(DEGMMA-co-MAA) were prepared by atom transfer radical polymerization of a mixture of methoxydi(ethylene glycol) methacrylate (DEGMMA) and tert-butyl methacrylate (t-BMA) with a molar ratio of 100: 13 from a PEO macroinitiator and a small molecule initiator, respectively, and subsequent removal of t-butyl group. PDEGMMA is a thermosensitive water-soluble polymer exhibiting a lower critical solution temperature in water at 25 °C. The cloud point of P(DEGMMA-co-MAA) in water can be readily tuned from 24 to 60 °C by changing the solution pH. The block copolymers dissolved molecularly in cold aqueous buffer solutions with a pH of 4.0 and underwent micellization when the temperature was raised to a critical point. Upon judiciously changing the solution pH by injection of a predetermined amount of a KOH solution, the block copolymer micelles were dissociated into the unimers, which subsequently reformed micelles at the same temperature in response to the addition of a predetermined amount of a HCl solution or heating to a higher temperature. These temperature- and pH-induced micellization/dissociation transitions were reversible. By continuously increasing temperature from 20 to 57 °C and simultaneously controlling the pH, three cycles of micellization and disassembly transitions of these block copolymers in aqueous solutions were realized, demonstrating the possibility of achieving on-demand micellization and dissociation transitions by combining temperature and pH triggers. Fluorescence spectroscopy studies showed that a hydrophobic fluorescence dye, Nile Red, can be repeatedly encapsulated by block copolymer molecules upon micellization and released upon dissociation of micelles under different combinations of pH and temperature.

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