面向碳捕集分离的离子液体基框架材料的定向合成及构效调控

How to cost-effectively capture CO2 from industrial flue gas and alleviate the greenhouse effect is a globe challenge. A lot of problems are related with the current amine scrubbing method, for example, evaporation/ degradation, severe corrosion, energy-intensive, which significantly limit their long-term application. There is an urgent need to develop efficient strategies to remove CO2 using alternative materials with high separation performance and energy efficiency. The project aim to synthesize the completely new ionic liquids - based porous frameworks with multiple CO2 separation function, which take advantages of the flexibility of ionic liquids and the excellent structure properties of the porous materials.The controlled synthesis, structural characterization, and CO2 adsorption properties of the ionic liquids frameworks will be system-depth investigated by ccombined methods of experiment, simulation and in situ spectral characterization. It will reveal how the spatial configuration and key functional groups of the ionic liquids build units; the complicated microscopic interaction of the synthesis system (such as hydrogen-bond, electrostatic and synergetic effect) affects the structures and properties of the synthesized materials. And the microscopic interaction of CO2 and the ionic liquids-based porous frameworks, the key factors to their performance, and the mutual restraint of synthesis - structure - performance will be also disclosed in these studies. The formed new understandings and methods will provide the indispensable theoretical guidance and technical support for the design and controlled synthesis of the alternative CO2 adsorbents and the ionic liquid-based frameworks with new structures and functions.

高效捕集CO2缓解温室效应是全球面临的重大挑战。传统醇胺吸收法能耗高，迫切需要开发低能耗、高性能的替代吸附剂及分离技术。本项目将离子液体的灵活性和框架材料优良的结构特性相结合，提出设计合成新型具有多重CO2分离功能的离子液体基框架材料的新思路，通过实验研究、模拟计算结合先进的原位光谱表征技术，从控制合成、结构表征、CO2吸附性能/机理三方面展开系统深入研究，获得离子液体结构单元的空间构型、关键功能基团及材料合成体系中复杂的微观作用（氢键、静电、多物种协同等）对其结构和性能的影响规律，研究框架材料的结构特性对传统功能离子液体/CO2微观相互作用机理（如氢键、阴阳离子协同、化学键合作用等）的影响规律及影响材料吸附性能的关键因素，阐明合成-结构-性能相互制约规律及调控机制，并为新一代经济高效分离CO2吸附剂&工艺的开发以及具有新型结构和功能的离子液体基框架材料定向设计及可控制备提供理论指导。

从工业烟气中捕集和回收CO2是缓解温室效应的重要策略之一。本项目针对CO2捕集分离的关键科学问题，在离子液体基多孔框架材料的设计合成、表征及多尺度构效关系方面取得了如下重要进展：1）通过硝基和胺基反应、氨基和原乙酸三甲酯缩合反应、氰基自聚、季胺化以及复分解等反应采用溶剂热、水热合成等方法合成了系列含咪唑、卟啉、偶氮、脒基等一种或多种功能基团的多孔离子框架材料；2）通过利用SEM/TEM、BET、XRD/XPS、EDS、IGA等手段对离子框架材料结构、CO2/N2吸附性能、CO2催化转化性能进行系统研究，揭示了多孔离子框架材料的合成-结构-性能多层次构效关系规律及调控机制。本项目发表期刊论文10篇，申请专利5项，项目团队成员积极参加国际/国内会议（16次），与多孔材料合成与表征领域的国际著名团队建立了深入的合作关系，取得的成果可为CO2的捕集分离以及离子框架材料合成新领域的开辟的提供科学支撑。