Cerium and Manganese Incorporated Zeolites as Catalysts for C-C Coupling Reactions

C-C coupling reactions are of high interest to synthetic chemists due to their ability to accomplish chemical transformations often involving value addition to the substrates. The high impact of the research in this area is evident by a Nobel Prize awarded to Richard F. Heck, Ei-ichi Negishi, and Akira Suzuki in the year 2010. This thesis outlines a research project in the area of C-C coupling reactions to synthesize industrially relevant products using substrate molecules typically small oxygenates, such as, acetic acid, and C2-C3 aldehydes. The focus is on the development of suitable catalysts to accomplish these transformations efficiently. Self C-C coupling of acetic acid, and propionaldehyde via ketonization and aldol condensation, respectively, are the reactions under investigation during the course of this thesis project. Acetone, and 2-methyl-2-pentenal are the desired products, which have a wide range of industrial applications. However, tendency of these molecules to form longer carbon chains via continuous coupling is a major drawback during these reactions. Therefore, a catalyst that is highly selective to the desired products and that can deliver competitive yields is needed. With this regard, novel materials containing cerium and/or manganese heteroatoms incorporated in the zeolite frameworks are tested as catalysts. The data show the presence of Ce³⁺, and Mn³⁺ heteroatom species in the crystalline zeolite framework, and these catalysts are active at low temperature during self-aldol condensation reaction as well as can deliver higher rates to the desired products during the C-C coupling reactions of small oxygenates tested.