鸟苷类超分子自愈性凝胶的愈合机理及性能调控

Supramolecular self-healing gels based on small molecular gelators have potential applications in the field of sensors, tissue engineering, wearable devices and so on, which will improve the lifetime of the devices and reduce replacement cost. However, the healing mechanisms of this kind of materials have not been well explored, and the present supramolecular self-healing gels are weak and fragile, which greatly blocks their practical applications. Herein, we proposed a test-tube brush self-healing model. Based on this model and our preliminary research work, a series of guanosine-based small molecular self-healing gelators with different self-assembly functional groups are designed and will be synthesized. The gelation properties, self-healing properties, structure-property relationship and self-assembly mechanisms of these novel self-healing gelators are going to be studied in detail to clarify the relationship between the structure of the gelators, the structure of the supramolecular aggregates and the self-healing properties. As a result, a reasonable self-healing mechanism model is expected to be established through molecular simulation. Moreover, we would like to control the mechanical properties and self-healing properties of the obtained supramolecular gels by employing guanosine-modified polymers and prepare both tough and self-healing gels for practical applications. The interactions between polymers and small molecular gelators will be revealed to further study the self-healing mechanisms of supramolecular gels. The research work will provide theoretical support for the application of supramolecular self-healing gels in the field of soft machines, soft devices etc., and will promote the development of Supramolecular Chemistry, Chemistry of Materials and other disciplines.

基于小分子胶凝剂的超分子自愈性凝胶在传感器、组织工程和可穿戴设备等不同领域具有潜在应用，可提高器件使用寿命，降低生产成本。目前此类胶凝剂均为偶然发现，其自愈合机理尚无系统研究；材料机械性能差，应用受限。本项目提出一种“试管刷”自愈合机理模型，并依此模型及本项目的前期研究工作，设计与合成一系列具有不同自组装基团的新型鸟苷类小分子自愈性胶凝剂。通过凝胶性能、自愈性能、构效关系和自组装机理研究，阐明胶凝剂的分子结构-超分子聚集体结构-自愈性能之间的作用规律，通过分子模拟与计算建立超分子自愈合机理模型。通过添加鸟苷修饰的高分子化合物，调控超分子凝胶的机械性能和自愈性能，探寻有实际应用性的自愈性凝胶软材料；通过建立高分子-小分子共组装模型，深化自愈合机理研究。本研究工作将为超分子自愈性凝胶在软机器、软器件等领域的应用提供理论支持，推动超分子化学、材料化学等学科的发展。

基于小分子胶凝剂的超分子自愈性凝胶在传感器、组织工程和可穿戴设备等不同领域具有.潜在应用，可提高器件使用寿命，降低生产成本。目前此类胶凝剂均为偶然发现，其自愈合机理尚无系统研究；材料机械性能差，应用受限。本项目在我们已有研究成果的基础上，设计与合成了一系列具有不同自组装基团的新型鸟苷类超分子凝胶。通过凝胶性能、自愈性能、构效关系和自组装机理研究，阐明了胶凝剂的分子结构-超分子聚集体结构-自愈性能之间的作用规律，通过分子模拟与DFT理论计算验证了本项目提出的“试管刷”自愈合机理模型。通过在鸟苷超分子网络中引入聚合物网络，首次设计开发了系列具有优异机械性能、超高拉伸性和广泛界面粘附性的超分子-聚合物双网络水凝胶和低共熔凝胶材料平台，并开发了此类材料在可拉伸能源存储设备器件、柔性可穿戴传感器、柔性电致变色设备以及高强度粘附剂领域的应用。相关研究的进展和突破，不仅设计制备出了系列多功能软材料，而且也为研发具有实用价值的新型分子器件提供新的思路，推动了超分子化学、材料化学等学科的发展。截至目前围绕本项目已在本领域国际高水平学术期刊上发表SCI 收录论文16篇，其中JCR一区TOP文章累计13篇，包括Angew. Chem. Int. Ed.；Energy Environ. Sci.; Coord. Chem. Rev.；Adv. Funct. Mater.；Appl. Catal. B ; Mater. Horiz.等；ESI高被引0.1%热点论文1篇。围绕本项目共获授权发明专利2项。