SBA-16负载手性M-Salen催化苯乙酮不对称加氢

在均相体系中，前手性酮不对称加氢获得了良好的催化效果。其催化剂大多是贵金属配合物，在反应过程中这些配合物难与底、产物分离，既不经济又造成严重环境污染。"均相催化剂-多相化"是解决这一问题的重要手段。本项目拟以SBA-16介孔分子筛材料作为载体，分别通过："原位合成法"、"自由配体"法、"瓶中造船"法等不同手段，将配位能力较强的手性Salen配体与钌、铑、钯、铱等贵金属配合物固载在SBA-16纳米的、三维的、规则的、大体积的超笼中,制备系列多相不对称加氢催化剂，并对其结构进行详细表征。以苯乙酮及其衍生物催化不对称加氢反应作为探针，考察载体、配体、中心金属等与底物的匹配能力；考察该类手性催化剂的合成工艺、结构性能及催化活性，寻找SBA-16负载型多相不对称催化剂合理的合成路线。

Homogeneous chiral catalysts have shown distinguished catalytic properties in asymmetric hydrogenation of prochiral ketones to optically active chiral alcohols. The precious metal complexes used as catalysts are difficult to separate from the substrate and productions, which is neither economic and causes serious environmental pollution. Therefore, increasing demand has been generated for the preparation of heterogeneous catalysts. SBA-16 is highly ordered porous silica with large mesopores arranged in body centered cubic (BCC) Im3m symmetry. Its large cages can accommodate metal complexes of large molecular size, whereas the smaller pore entrances may prevent leaching of the metal complex confined in the mesoporous cages. In this program, the cage-like mesoporous silica SBA-16 will be synthesized and introduced in asymmetric catalysis system as support. Various of heterogeneous catalysts will be synthesised through several strategies and be characterized detailedly. In the whole study, the catalytic asymmetric hydrogenation of acetophenone and its derivatives acts as a probe reaction. The match between the central metal, ligand, carrier and the substrate, and the synthesis process, the structural properties and the catalytic activity of the chiral catalyst will be investigated. This program aims to discover the reasonable synthetic route of SBA-16 supported heterogeneous asymmetric catalyst.