聚合物组装体为交联剂制备力响应水凝胶

Mechano-responsive polymer materials have found significant applications in stress mapping, materials failure analysis, catalysis, and self-healing. While the traditional mechano-responsive hard materials have great limitation in the field of soft robotics and flexible devices, mechano-responsive hydrogels are promising candidates to overcome these problems. However, current strategies for mechano-responsive hydrogel could not simultaneously solve the problems that mechanophores are not soluble in water and hydrogels are generally mechanically weak.This proposal aims to develop a general strategy to construct robust and superstretchable mechano-responsive hydrogels. In this proposal, we plan to combine the “living”/controlled radical polymerization and amphiphilic copolymer self-assembly to prepare mechano-responsive assemblies, and use them as the crosslinker for mechano-responsive hydrogels. The incoorporation of mechano-responsive polymer assemblies not only brings about mechano-responsive properties, but endow the hydrogels with supertough and superstrechable properties, which is promising to realize their application in visualized mapping the stress of hydrogel actuators. This project would provide a new universal strategy for constructing supertough and superstrechable mechano-responsive hydrogels, which would be of great importance to the fields of stress mapping, failure analysis and self-healing.

力响应聚合物材料在应力分布成像、材料失效分析、催化以及自修复等领域有重要的应用。传统力响应硬材料在软体机器人、柔性器件等领域的应用受到很大限制，力响应水凝胶有望克服这些困难。然而，现有的力响应水凝胶构筑策略难以同时解决力敏团在水相难溶和水凝胶模量低的双重问题。本项目拟发展一种通用的制备策略构筑超韧超弹力响应水凝胶。项目拟结合高分子“活性”/可控聚合技术与两亲共聚物自组装技术，制备力响应组装体，并以这些组装体为交联剂制备力响应水凝胶。力响应聚合物组装体的引入不仅带来力响应性质，还赋予水凝胶超韧超弹性质，从而有希望实现其在驱动器受力分布的可视化成像。本项目为超韧超弹力响应水凝胶的构筑提供了新的通用策略，对软物质的应力分布成像、失效分析及自修复等领域有重要意义。

聚合物组装体为交联剂可实现具有超弹性的增韧水凝胶的制备，且胶束的疏水核可同时解决难溶功能组分在水凝胶中的分散问题。本项目原计划利用胶束交联策略设计制备力响应水凝胶。根据该计划，我们发展了聚合诱导自组装策略实现纳米结构可控的聚合物组装体交联剂的高浓度制备，并将其用于制备胶束交联水凝胶，从而成功实现了力学性能优异的胶束交联水凝胶的通用制备。评估了组装体浓度、尺寸、成核链段玻璃化转变温度对胶束交联水凝胶机械性能的影响，建立了胶束交联剂结构与水凝胶机械性能的构效关系，为设计制备力响应胶束交联水凝胶材料提供了指导原则。设计制备了螺吡喃基小分子交联剂，利用聚合诱导自组装实现了力响应组装体的制备，并成功实现了力响应水凝胶的制备。但得到的力响应水凝胶机械性能弱，水凝胶的力响应传感未能良好实现。项目执行期间，共以第一作者/通讯作者在Science China Chemistry、Chemistry of Materials、Macromolecules、Polymer Chemistry上共发表项目资助论文4篇，获授权专利1项，培养硕士研究生6人。