CAS: Elucidating Trends in Earth-Abundant Metal Catalyzed Dehydrocoupling

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With the support of the Chemical Catalysis program in the Division of Chemistry, Ryan J. Trovitch of Arizona State University is studying the development of sustainable catalysts that feature abundant, inexpensive metals that do not have known toxicity to the environment. These catalysts will be deployed to synthesize value-added chemicals and polymers in a more efficient manner. This project aims to establish trends that relate to optimal catalyst structure. This information will be used to guide the development of catalysts based on abundant metals for a variety of chemical transformations. The initial reactions of interest will target molecular precursors critical to semiconductor manufacturing. This approach will then be expanded to explore the preparation of anti-corrosion and anti-graffiti coatings for the construction and transportation sectors, compounds for chemical vapor deposition, quantum dot precursors, and reagents for organic synthesis. The broader impacts of this project include the planned development of research-driven undergraduate laboratory experiment(s) and the creation of a manual for sustainable general and inorganic chemistry.With the support of the Chemical Catalysis program in the Division of Chemistry, Ryan J. Trovitch of Arizona State University is studying the development of highly-active manganese, iron, cobalt, and nickel catalysts for the dehydrocoupling of main group hydrides. Physical inorganic techniques will be relied on to elucidate trends in electron count, metal oxidation state, geometry, chelate coordination, and ligand redox activity that correlate with catalyst efficiency and lifetime. This effort will begin with the preparation of arene diimine compounds that are structurally related, yet electronically distinct from popular pyridine diimine compounds. As isostructural series and isoelectronic pairs are characterized, their ability to mediate the dehydrocoupling of amines and silanes will be evaluated. The most effective catalysts will be then used to prepare industrially-relevant aminosilane monomers and polymers. Catalysts developed during this project will also be screened for main group element dehydrocoupling reactions that have not been previously achieved. Applications will include the preparation of chemical vapor deposition and atomic layer deposition precursors that feature N-Ge, N-Al, and Ga-P bonds, quantum dot synthons that feature P-Si and P-Ge bonds, and reductive functionalization reagents that feature B-Si and Al-Si bonds. Overall, this project has the potential to expand the known scope of main-group element dehydrocoupling chemistry and elucidate halogen-free synthetic pathways that can be used to prepare a versatile set of products. The broader impacts of this project include the potential for positive societal outcomes in the fabrication of quantum dots and the distribution of effective catalysts to members of the synthetic community. A sustainable general and inorganic chemistry laboratory guide for post-secondary educators will be developed and undergraduate students will evaluate the sustainability of competing synthetic transformations through the newly developed coursework.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.