Atom-Efficient Heteroatom Transformations Mediated by f-Element and d(0) Catalysts

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With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Tobin Marks of Northwestern University is discovering, understanding, and optimizing, f-element and d(0)-transition metal catalysts for three different types of critical organic reactions. It is estimated that catalysis underpins approximately 35% of the U.S. GDP, producing coatings, fertilizers, fuels, plastics, pharmaceuticals, medical garments and equipment, and other chemicals on a vast scale. In the future, catalytic transformations must be more energy and resource efficient, non-toxic, non-polluting, and employ low-cost, earth-abundant metals in more selective, sustainable, and economically competitive technologies. Professor Marks and his research group are addressing these important challenges with the development of f-element and d(0) catalysts that advance new ways to build and modify organic molecules. These activities are also serving to educate young scientists to attack global-scale problems, while conducting forefront research across broad disciplinary fields. Projects funded by this award involve a transdisciplinary, educationally rigorous combination of catalyst creation, catalyst evaluation, and understanding the pathways by which catalytic products are formed. These activities combined with a highly interactive research group environment, provide excellent training/mentoring for graduate, undergraduate, and postdoctoral scholars bound for industrial, national laboratory, or academic careers, with special emphasis on participation by women and underrepresented minorities.The research program supported by this award is configured around three highly-integrated exploratory, hypothesis-driven themes capitalizing on the unique properties of earth-abundant lanthanide, actinide, and early transition metal complexes. In the first, a remarkably rapid and selective reduction process for carbon-element multiple bonds using simple lanthanide catalysts and easy to handle boron compounds is being investigated for new synthetic applications to facilitate access to natural products, pharmaceuticals and fine chemicals. In the second theme, the position of catalytic rare earth metals in the periodic table is being used to steer reaction outcomes. When applied to pyridine molecules, which are important for drugs and fine chemicals, large lanthanides lead to a change in the pyridine double bond structure whereas small lanthanides lead to substitution on the pyridine periphery. In the third theme, the tolerance of zirconium olefin polymerization catalysts towards the copolymerization of monomers with amine, phosphine and thioether functional groups is being investigated and the properties of the resulting materials explored. The broader long term scientific impact of this research includes the potential provide new routes to build-in surface anti-bacterial, anti-viral, and anti-fungal characteristics for disposable PPEs and even hospital clothing and face masks.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.