通过开环交替共聚合成可降解聚酯的性能中两个单体之间的相互作用,ACS Macro Letters

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通过开环交替共聚合成可降解聚酯的性能中两个单体之间的相互作用
ACS Macro Letters ( IF 5.1 ) Pub Date : 2023-04-17 , DOI: 10.1021/acsmacrolett.3c00104
Sumin Lee ₁ , Woo Hyuk Jung , Minseong Kim ₁ , Dong June Ahn , Byeong-Su Kim ₁

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环酐和环氧化物的开环交替共聚 (ROAC) 已成为一种强大的策略，可通过两种不同的结构单元的组合生产具有多种结构的可降解聚酯。在这项工作中，我们利用了环酐和功能性环氧化物的有机催化 ROAC，t-butyl glycidoxy acetate，然后进行酸性脱保护以获得带有羧酸悬垂物的可降解聚酯。为了研究单体之间的相互作用，使用二甘醇酸酐和戊二酸酐作为环状酸酐来制备两种聚酯。特别是，研究了环酐中氧杂原子对含羧酸聚酯性能的影响。将氧杂原子引入环状酸酐显着影响了它们在水溶液中的热性能和 pH 依赖性自缔合行为。此外，分子动力学模拟表明，氢键的数量和类型在聚合物在溶液和本体状态下的自缔合行为中起着至关重要的作用。

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Tailoring the Interplay between Two Monomers in the Properties of Degradable Polyesters Synthesized via Ring-Opening Alternating Copolymerization

Ring-opening alternating copolymerization (ROAC) of cyclic anhydrides and epoxides has emerged as a powerful strategy to produce degradable polyesters with a diverse array of structures from the combination of two distinct building blocks. In this work, we exploited the organocatalytic ROAC of cyclic anhydrides and a functional epoxide, t-butyl glycidoxy acetate, followed by acidic deprotection to access degradable polyesters with carboxylic acid pendants. To study the interplay between monomers, diglycolic anhydride and glutaric anhydride were used as cyclic anhydrides to prepare two polyesters. In particular, the effects of the oxygen heteroatom in the cyclic anhydrides on the properties of the carboxylic acid-containing polyesters were investigated. The introduction of the oxygen heteroatom into the cyclic anhydrides significantly influenced their thermal properties and pH-dependent self-association behavior in an aqueous solution. Furthermore, molecular dynamics simulations elucidate that the number and type of hydrogen bonds play a crucial role in the self-association behavior between the polymers both in the solution and bulk states. The findings of this study highlight the importance of the interplay between monomers in the design of functional polyesters with tunable properties.

更新日期：2023-04-17

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