A new supramolecular catalyst utilizing π-related interactions for the assembly has been developed. By introducing π-unit to salen complexes to induce assembly through intermolecular π-related interactions, enhanced catalytic activity and stereoselectivity of the salen complexes were observed. It has been proven that some salen complexes catalyze reactions through dual activation of substrate and reactant (nucleophile) by a separate catalyst each. The intermolecularly closely placed catalytic sites in the assembled salen complexes would cooperatively function to efficiently induce the dual activation of substrate and reactant by the separate salen complex each. Since the structure and arrangement of the π-unit significantly affected the catalytic activity and selectivity, assembly property of the salen complexes certainly play an important role in the catalysis. To obtain mechanistic insights into the assumed self-assembly catalysis, some control experiments, NMR study, FE-SEM analysis, kinetics study, and mass spectroscopic analysis were conducted. The mechanistic studies supported the assumed assembly pathway. Highly efficient and stereoselective hydrolytic epoxide ring-opening reactions have been accomplished by the supramolecular Co(III)-salen complexes. Applications of the supramolecular catalyst system to other salen complex-catalyzed reactions were also investigated. Some unique reactivities of the supramolecular salen complexes were observed in the reactions. The scope of salen complex-catalyzed reactions has been expanded by the present catalyst systems.

Self-assembly salen complexes utilixing π-related interactions for efficient cooperative<i> </i>catalysis

2019 Spring National Meeting

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Self-assembly salen complexes utilixing π-related interactions for efficient cooperative catalysis