响应性表面活性剂调控的DNA耗散组装体的构筑及性能研究

The use of dissipative self-assembly to construct fuel dependent, energy consuming and dynamic non-equilibrium dissipative assemblies is of great significance for the development of intelligent bionics and environmental protection materials. Dissipative self-assembly has also become a research hotspot in the fields of material chemistry, biomedicine science, environmental chemistry and physical chemistry. In this project, a novel magnetic surfactant containing dynamic hydrazone bond will be designed, which dissipative self-assembles with biocompatible DNA to construct the magnetically dissipative self-assemblies. By virtue of the dynamic reversibility from surfactant molecules and the DNA molecular enzymatic responsiveness, various chemical fuel/energy consumption mechanism will be introduced into the dissipative assemblies of surfactant/DNA. They could serve as wonderful choices for preparing intelligent, feedback regulated and multi-responsive functional materials including bionic materials, drug carriers and phase transfer reactors. The relationship between the molecular structure of building blocks in dissipative self-assemblies and the chemical fuels/energy consumption mechanism will be deeply explored. Responsive surfactant/DNA assemblies constructed by dissipative self-assembly have important implications for the construction of high-energy, non-equilibrium and intelligent functional materials.

利用耗散自组装构筑燃料依赖、能量消耗、动态非平衡的耗散组装体对于发展智能仿生和能源环保类材料有重要的意义，耗散自组装也成为材料化学、生命医药、环境化学和物理化学领域的研究热点。本项目设计含有动态酰腙键的新型磁性表面活性剂，与生物相容性良好的DNA进行耗散自组装研究，构筑具有磁响应性质的耗散组装体。借助表面活性剂分子的动态可逆性和DNA分子的酶响应特性，多种化学燃料/能量消耗机制被引入到表面活性剂耗散组装体中，筛选出具有智能性、反馈调节、多重响应机制的耗散组装体构筑智能型功能材料，如仿生材料、药物运载体和相转移反应器等。重点探究耗散自组装体各构筑基元分子结构与耗散组装体的能量消耗机制之间的关联。利用耗散自组装方法构筑的响应型表面活性剂/DNA组装体对于构建高能量、非平衡、智能型功能材料有十分重要的启示作用。

本项目从应用需求出发，着重于设计与挑选自组装分子或材料。项目涉及到信息加密、催化氧化、DNA自发捕捉释放、电极材料构筑等多方面应用需求，因而该工作着力于构筑单元的设计、合成与组装过程。项目主要开展了以下几个方面的工作：1）挑选具有响应性质的表面活性剂分子、生物相容性良好的生物分子、功能性小分子进行研究，进而构筑了功能性荧光复合材料、催化复合材料和电极复合材料。2）从相互作用力的角度进行分析，协同运用静电相互作用、疏水相互作用、氢键相互作用、动态共价键等多种作用力，辅以自组装、水热合成等方法构筑功能材料，通过一系列表征测试分析功能材料形成的原理且分析功能组装体的性质与功能。3）挑选有潜力的静态组装体，辅以能量输入/能量耗散设计模式，构建瞬态组装体并对其相关影响因素进行探究，总结出规律，设计出功能性瞬态组装材料。