生物质碳酸钙基“受阻”路易斯酸碱对(FLP)的构建及其催化C=N键氢化机理的研究

催化加氢作为有机合成中的一种有效还原手段，具有反应易于控制、产物收率高、原子经济性高等特点。目前，催化加氢技术主要依赖贵金属材料催化，而研发高效、绿色的新型非贵金属催化加氢体系仍是一大挑战。相比于贵金属材料，“受阻”路易斯酸碱对(Frustrated Lewis Pairs, FLPs)在催化加氢过程中具有环境友好，无重金属残留等优势，符合绿色化学的要求。本项目申请团队早期研究发现，表面富含羟基的生物质碳酸钙能够有效的吸附游离的H2分子。考虑到生物质碳酸钙的特殊性质，本项目拟用生物质碳酸钙表面羟基作为路易斯酸性位点，强σ给电子能力的氮杂环卡宾(NHC)作为路易斯碱性位点，原位调控新型的生物质碳酸钙基异相FLPs的结构，研究该FLPs结构与催化C=N键加氢反应性能的构效关系。本申请项目通过对生物质碳酸钙表面的合理修饰使其结构功能多样化、应用多元化，为研发新型的催化加氢体系提供理论依据。

As an effective reduction method in organic synthesis, the development of efficient catalytic hydrogenation system is still challenging. Compared to noble metal catalysts, the frustrated Lewis pairs has the advantages of environmental friendliness, no heavy metal residue, which conforms to the requirements of green chemistry . In this proposed project, a new heterogeneous bio-CaCO3 based-FLPs catalysis with hydroxyl group and N-heterocyclic carbene (NHC) would be constructed and the structure-activity relationship for hydrogenation of unsaturated C=N bonds would be studied. This proposed project intends to make the bio-CaCO3 more diversification in structure and application, which would provide some directive value for the development of new catalytic hydrogenation system.