基于超分子作用的形状记忆弹性体的本征自修复行为及其机理研究

In the application, shape memory polymers mostly have low reusability, aging or even damage during cyclic using, decreased recovery rate, and poor structural stability, etc., which affect the service life and the scope of application. If the shape memory polymers possess self-healing properties, the service life can be effectively extended. The existing self-healing shape memory polymer has the problems of lack of systematic molecular structure design theory support, complicated preparation process, difficulty in realizing intrinsic self-healing or unclear of the healing mechanism. Based on this background, this project studies the intrinsic self-healing behavior and its mechanism of the shape memory elastomer based on supramolecular interactions. It is proposed to design and prepare shape memory elastomers with intrinsic self-healing properties starting from the construction of supramolecular polymers. At the same time of material preparation and performance analysis, a complete molecular dynamics model was established to explore the relationship between its aggregation structure, self-healing mechanism and shape memory behavior. Solve key technical problems such as damage reduction and rapid self-healing of the shape memory elastomers. Establish a molecular structure design theory that improves the recovery rate and service life of shape memory elastomers and broadens their range of application. The study of this proposal will provide powerful theoretical and experimental support for the design and fabrication of intrinsic self-healing shape memory elastomers.

形状记忆聚合物在应用中大多存在重复使用率低、循环使用时出现老化甚至破坏、回复率下降、结构稳定性变差等现象，影响材料的寿命及使用范围。如赋予其自修复性能，则可有效延长材料使用寿命。现有自修复形状记忆聚合物存在缺乏系统的分子结构设计理论支撑、制备工艺繁琐、难以实现本征自修复或修复机制不明确等问题。本项目基于该背景，进行基于超分子作用的形状记忆弹性体的本征自修复行为及其机理研究。提出从构建超分子聚合物出发，设计和制备具有本征自修复性能的形状记忆弹性体。在完成材料制备和性能分析的同时，建立完善的分子动力学模型，探究其聚集态结构、自修复机制以及形状记忆行为的关系，解决形状记忆弹性体材料在使用过程中的损伤降低和快速修复等关键技术问题，建立系统的提高形状记忆弹性体的回复率及使用寿命、拓宽其使用范围的分子结构设计理论。该项目的研究将为设计和制备本征自修复型形状记忆弹性体提供有力的理论和实验支撑。

本项目针对形状记忆聚合物在应用中大多存在重复使用率低、循环使用时出现老化甚至破坏、回复率下降、结构稳定性变差等问题，开展了基于超分子作用的形状记忆弹性体的本征自修复行为及其机理研究。首先完成了具有本征自修复性能的超分子形状记忆弹性体的材料设计，通过锌离子与端羧基聚丁二烯、聚苯乙烯-乙烯基吡啶配对，成功制备了基于金属配位超分子作用的自修复聚丁二烯橡胶。并在该橡胶体系中添加零维纳米材料氧化碳纳米洋葱，增强了橡胶的机械性能与自修复性能，实现了材料功能的多元化和寿命的延长；研究了基于超分子作用的形状记忆弹性体的本征自修复性能的驱动方法，实现了对自修复性能和形状记忆性能的优化控制，所制备的超分子弹性体具备形状记忆辅助自修复效应，该效应可显著缩短自修复所需时间；进一步建立了形状记忆弹性体自修复性能的量化评价方法和基于超分子体系微结构自组装理论的形状记忆自修复材料多功能材料设计方法。研究成果为形状记忆辅助自修复的微观体系结构提供了设计依据，对推动智能多功能材料的推广应用具有重要意义。基于本项目的研究内容，在Polymers、Polymer Degradation and Stability等高水平期刊上发表SCI收录论文3篇，申请发明专利1项，参加第32届自适应结构与技术大会（ICAST2022）及国际先进材料与制造工程学会年会（SAMPE2022）等国际会议并做口头报告，培养硕士研究生4名，本科生若干名，协助培养博士研究生1名。

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