Experimental and Computational Studies of Bifunctional Organometallic Catalysis

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With the support of the Chemical Catalysis Program in the Division of Chemistry, Professors Douglas B. Grotjahn and Andrew L. Cooksy of San Diego State University are performing research aimed at determining the best catalysts for new reactions that can be used to make organic compounds of interest for a variety of applications, including pharmaceuticals, materials, and biology. To accomplish this, many catalysts that contain a metal and a larger non-metal portion (ligand) will be made and tested, to determine what combinations of metals and ligands will yield the best performing catalysts. In addition, fundamental studies of how the catalysts operate on the molecular level will be performed. This grant will support the training of several young investigators in the field of catalysis. Because catalysis accounts for a third of global GDP and a majority of chemical products and chemical processes, the discovery of new or improved catalysts for organic reactions and new mechanisms has great practical importance, contributing to economic development and recovery. As in the previous grant period, practical catalysts will be developed and improved. Also, to broaden public understanding of catalysis, the PIs and the graduate students will introduce the concept into an existing and highly successful high school outreach program.With the support of the Chemical Catalysis Program in the Division of Chemistry, Professors Douglas B. Grotjahn and Andrew L. Cooksy of San Diego State University will employ design principles of Nature’s enzymes, particularly hydrogen bonding and proton transfer, to accelerate (often by more than 1000-fold) organometallic catalysis and reactions by new mechanisms. Ligands containing proton-donating or hydrogen-bonding groups will be synthesized and combined with a variety of metal precursors to form their metal derivatives for catalysis. Interactions of these pendant groups with nonpolar and polar reactants, intermediates, or transition states are expected to create faster catalysts. The focus will be mostly on waste-free addition or isomerization reactions, with several goals: (1) integrate the use of computer-based molecular predictions before and after catalyst discovery; (2) build and apply a toolbox of alkene isomerization catalysts; (3) use ligands to enable X-H activation; and (4) develop catalysts for addition reactions. The project will include significant one-on-one training in modern techniques of organic and organometallic chemistry, including NMR spectroscopy, catalysis screening, and computation. The proposed research will add new mechanistic insight to our picture of bifunctional catalysis, using complementary experimental and computational studies to allow the design of better catalysts and chemical processes.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.