超分子自组装能够在纳米乃至分子尺度上对材料的结构和性能进行有效的调控，是一条极具前景的“自下而上”型的材料制备手段。然而，如何通过分子自组装，在宏观尺度上可控制备结构化的超分子材料尚较困难。主要原因是由于从分子到宏观尺度经历了多个尺度的跨越，导致整个材料形成过程很难加以控制，从而无法直接组装出所预期的宏观材料结构。本项目拟从一基于腙键的模块化超分子凝胶体系入手，以反应扩散型分子自组装为手段，对在宏观尺度上可控制备结构化超分子凝胶进行系统的研究。通过在宏观尺度上控制腙型凝胶因子前驱体（醛型和肼型分子）在空间中的扩散和反应过程，使得腙型凝胶因子在所设定的宏观区域内生成和组装，最终，制备得到宏观结构化超分子凝胶。本项目还将通过建立反应扩散模型来揭示所涉及的结构化超分子凝胶的形成机理。该项目的成功实施将为宏观结构化超分子材料的可控制备开辟一条新方法，为进一步拓展超分子材料的功能和应用奠定基础。

Supramolecular self-assembly is a useful “bottom-up” approach for materials fabrication, which can control the organization of materials at the nanoscale or even at the molecular level. However, it remains a challenge to control the formation of structured materials at the macroscopic length scale through molecular self-assembly. The main reason leading to this issue is the poor controllability over such a multilevel process from small molecules to the macroscopic world. In this project, the applicant attempt to develop a reaction-diffusion based self-assembly approach, relying on a hydrazone-based modular supramolecular hydrogel system, for the fabrication of macroscopically structured supramolecular hydrogels. Upon controlling the spatial distribution of the reaction and diffusion of the hydrazone gelator precursor molecules (aldehyde and hydrazide, respectively) at the macroscopic level, the hydrazone gelators are formed at the interested macroscopic areas and ultimately self-assemble into the macroscopically structured supramolecular hydrogels. Moreover, a reaction-diffusion model will be developed to understand the formation mechanism of the macroscopically structured hydrogels. The accomplishment of the planed goals in this project will provide a new approach for the fabrication of macroscopically structured supramolecular materials, and pave the way towards unlocking more enticing functions and applications of supramolecular materials.