本征可拉伸自修复全水凝胶超级电容器制备与性能研究

Flexible supercapacitors are one important kind of energy storage devices for stretchable self-healing electronics, including wearable electronics, bionic prostheses, biomedical electronics and soft robots. However, it remains challenging to achieve synergistic regulation of the mechanical stretchability, self-healing ability and electrochemical performance of flexible supercapacitors to meet the demands of stretchable self-healing electronics. In this project, we will try to solve this problem by the fabrication of all-hydrogel-based supercapacitors, i.e., employing hydrogels as both electrodes and the electrolyte. To begin with, highly stretchable, well self-healable and highly electrochemically active hydrogel electrodes and electrolytes will be prepared via a systematic approach combining the cross-linked network structure, covalent bond and dynamic non-covalent interaction and dual charge storage mechanism. Then, all-hydrogel-based supercapacitors will be assembled using the resultant high-performance hydrogel electrodes and the electrolyte. The performance of the supercapacitors will be optimized through synergistically tuning each hydrogel component layers. It is anticipated that supercapacitors with high stretchability, high self-healing efficiency and excellent electrochemical performance can be fabricated. Finally, an optimizing strategy from the synergistic point of view will be established and the stretching and self-healing mechanism will be revealed. In conclusion, this project has significant values for promoting the development of stretchable self-healing electronics, both in terms of scientific research and industrial applications.

柔性超级电容器作为可穿戴电子设备、仿生假肢、生物医药电子及软体机器人等可拉伸自修复电子产品的关键储能电子元件，实现其力学拉伸性、自修复能力及电化学性能的协同调控以满足可拉伸自修复电子的发展需求，是该领域亟待解决的关键科学问题。本项目拟以超级电容器电极层与电解质层为突破口，以水凝胶为研究对象，通过水凝胶结构设计，引入交联网络结构、共价键与动态非共价作用及双重电荷存储机理，制备高度可拉伸、高效自修复及高电化学活性的水凝胶电极与电解质材料，并组装成全水凝胶超级电容器。通过解决各功能层的性能协同调控问题，实现整个器件性能的优化，从而构建高度可拉伸、高效自修复及电化学性能优异的超级电容器。建立材料与器件性能协同调控策略，进一步揭示拉伸与自修复机理。本项目的开展对于可拉伸自修复电子的发展具有重要科学意义与应用价值。

可穿戴电子在人机交互、人工智能、健康医疗等领域具有广阔的应用前景。为了实现可穿戴电子产品与人体器官的紧密贴合，增强其耐用性，需要其具有良好的拉伸性与自修能力。为了满足未来可穿戴电子拉伸自修复的发展需求，亟需开发与之匹配的拉伸自修复的储能器件。电极与电解质作为储能器件的基本组成部分，对器件性能具有巨大的影响。因此，设计开发新型电极及电解质，调控其力学拉伸性、自修复能力及电学化性能，构筑拉伸自修复高容量的储能器件是可穿戴电子领域亟待解决的关键科学问题。.为了解决上述问题，本项目以导电水凝胶为研究对象，通过交联网络结构设计及动态非共价键作用开发水凝胶电极与电解质，协同调控力学拉伸性、自修复能力。进一步组装成储能器件，通过解决电极与电解质功能层的拉伸自修复，结合器件结构优化，实现整个储能器件的拉伸、自修复与高容量。最后，揭示拉伸自修复机理。首先，建立了双添加剂诱导物理交联策略，实现了PEDOT:PSS的凝胶化，构建了一类新型自支撑的导电聚合物水凝胶电极。基于PEDOT:PSS水凝胶电极构筑了自支撑高弹性全凝胶超级电容器，该器件表现出非常高的比电容（≈177 mF cm-2）及出色的形变能力。然后，通过多重交联网络结构设计策略，开发了一类新型水凝胶电解质。借助多重交联网络拉伸过程中对应力的耗散作用及动态非共价键的可逆性，实现了水凝胶电解质拉伸性与自修复能力的协同调控，其拉伸率高达2000%，自修复效率约为90%。进一步通过原位沉积技术，构筑了互锁一体式超级电容器，该器件同时表现出优异的拉伸性（≈1060%）、高自愈合效率（≈80%）及高的比电容（109 mF cm-2）。采用印刷技术，制备了PEDOT:PSS/MXene/Ag网格柔性透明三元复合电极，进一步构建了柔性透明双功能电容式传感器，成功集透明度、储能及传感于一身，实现了器件的多功能化集成。.成果解决了若干制约柔性可穿戴电子发展的瓶颈问题，为设计制备拉伸自修复储能材料与器件提供了可行的技术方案与理论指导，为可穿戴电子的发展奠定了基础。