富含氮杂环卡宾前体基元的大环化合物的设计、合成及在二氧化碳固定化中的应用研究

当代温室气体排放已经到达临界值，二氧化碳（CO2）作为人类活动最主要排放的温室气体被视为重要污染物进行控制。CO2的化学固定化以其为C1底物取代石油化工原料合成新的化学品，被视为实现CO2减排乃至负排放的重要途径。CO2化学固定化的温和、绿色、高效策略是当今化学及环境科学的前沿研究领域。本项目的提出结合氮杂环卡宾（NHC）化合物在CO2固定化中的应用与超分子化学中的大环化合物研究两个前沿领域，计划设计合成一系列含有多个NHC生成位点的大环化合物，利用NHC的种类和取代基的不同调控其反应活性等性能，同时利用多种桥连基团的协同作用，实现对大环化合物及其可能生成的的二氧化碳加合物、酸式碳酸盐或卡宾-金属配合物构象的调控，利用大环化合物所具有的特定空腔结构和独特的化学环境，以其作为分子反应器，以期实现后继的CO2固定化研究。该研究有可能为CO2固定化提供新的思路和途径。

While greenhouse gases emissions are reaching alarming levels, it have been attached great importance to CO2 emission control. As the ultimate waste of the intensive utilization of carbon resources. CO2 fixation with chemical reaction, namely utilizing CO2 as a C1 building block to produce platform chemicals as an alternative to petrochemistry has a double advantage of reusing CO2 while sparing fossil resources and avoiding CO2 emissions from their use. The study of mild, green and effective method to fix CO2 is the front field of chemical and environmental sciences. The proposal herein will combine two research fileds: (1) using N-heterocyclic carbene (NHC) for CO2 fixation; (2) supramolecular macrocycle chemistry. The study will focus on the design and synthesis of new macrocyclic compounds with multi NHC precusor (NHCH+) units. The macrocycle compound property (e.g. reaction activity) control will be realized with the introduction of NHCH+ with different types and linkage groups. Different bridged units will control the conformations of multi-NHCH+ macrocycle compounds, also its NHC-CO2 adducts, hydrocarboxlate (NHCH+-HCO3-) and NHC-metal (NHC-M) complexes. It is expected that the macrocyclic structrues have the possibility to provide their unique cavities as the molecular reactors for CO2 fixation reaction. The study will develop new strategies and methods for CO2 fixation.