Hydrolysis-Driven Viscoelastic Transition in Triblock Copolyether Hydrogels with Acetal Pendants,ACS Macro Letters

当前位置： X-MOL 学术 › ACS Macro Lett. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Hydrolysis-Driven Viscoelastic Transition in Triblock Copolyether Hydrogels with Acetal Pendants
ACS Macro Letters ( IF 5.1 ) Pub Date : 2021-08-05 , DOI: 10.1021/acsmacrolett.1c00413
Jinsu Baek ₁ , Seyoung Kim ₂ , Iloh Son ₁ , Soo-Hyung Choi ₂ , Byeong-Su Kim ₁

Affiliation

While the hydrolytic cleavage of ester groups is widely exploited in degradable hydrogels, the scission in the midst of chain backbones can bring dramatic changes in the mechanical properties of the hydrogels. However, the predictive design of the mechanical profile of the hydrogels is a complex task, mainly due to the randomness of the location of chain scission. To overcome this challenge, we herein present degradable ABA triblock poly(ethylene oxide)-based hydrogels containing an A-block bearing acetal pendant, which provides systematically tunable mechano-temporal properties of the hydrogels. In particular, hydrophobic endocyclic tetrahydropyranyl or exocyclic 1-(cyclohexyloxy)ethyl acetal pendants are gradually cleaved by acidic hydrolysis, leading to the gel-to-sol transition at room temperature. Most importantly, a series of dynamic mechanical analyses coupled with ex situ NMR spectroscopy revealed that the hydrolysis rate can be orthogonally and precisely tuned by changing the chemical structure and hydrophobicity of acetal pendants. This study provides a platform for the development of versatile degradable hydrogels in a highly controllable manner.

中文翻译：

缩醛侧链三嵌段共聚醚水凝胶中水解驱动的粘弹性转变

虽然酯基的水解裂解在可降解水凝胶中被广泛利用，但链骨架中间的断裂可以给水凝胶的机械性能带来巨大的变化。然而，水凝胶力学特性的预测设计是一项复杂的任务，主要是由于断链位置的随机性。为了克服这一挑战，我们在此提出了可降解的 ABA 三嵌段聚（环氧乙烷）基水凝胶，该水凝胶含有带有 A 嵌段的缩醛侧链，它提供了水凝胶的系统可调的机械时间特性。特别是，疏水性内环四氢吡喃基或外环 1-(环己氧基)乙基缩醛侧基通过酸性水解逐渐裂解，导致室温下凝胶到溶胶的转变。最重要的是，一系列与非原位核磁共振光谱相结合的动态力学分析表明，水解速率可以通过改变缩醛侧链的化学结构和疏水性来正交和精确地调节。该研究为以高度可控的方式开发多功能可降解水凝胶提供了一个平台。

更新日期：2021-08-17

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11