RUI: The Role of Engineered Ligands in Putative Homogeneous Catalysis: Supporting a Homogeneous Catalyst or Modulating Nanoparticle Formation

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Emerging technologies such as the ability to convert carbon dioxide (CO2) into useful chemicals and the ability to use oxygen from the air as a reagent in chemical synthesis rely on catalysts that can speed up reaction rates and control which products are formed (selectivity). Catalysts can change structure and properties during a chemical reaction. The initial state of the catalyst may be known however, in general, far less is known about how catalysts might change over time under working conditions. Professor Margaret Scheuermann of Western Washington University is identifying and investigating catalysts structure while the catalyst is working. The team led by Professor Scheuermann is using both existing and newly developed techniques to characterize the resultant structures and understand their catalytic properties. The findings are giving insight into the role and significance of catalyst structure. The undergraduates and masters level students participating in this project are developing research skills that they will apply later as members of the STEM workforce. With funding from the Chemical Structure, Dynamics, and Mechanisms B (CSDM-B) Program of the Chemistry Division, Professor Margaret Scheuermann of Western Washington University is working to identify putative homogeneous catalytic systems in which nanoparticles are formed, characterize the particles, and attempt to discern whether the particles are an inactive decomposition product, a pre-catalyst/off-cycle species, or an active catalyst. The studies are focused on easily reduced late metals with highly engineered polydentate ligands that are known precatalysts for biomass deoxygenation, CO2 hydrogenation/formate dehydrogenation, and aerobic oxidation reactions. In addition to employing established tests for identifying and assessing nanoparticles in putative homogeneous catalysis, the Scheuermann group is developing new tests based on centrifugal forces and non-reactive polymers to gain insight as to whether the observed catalysis is best explained by solution chemistry (molecular species or small clusters), surfaces (bulk solid or nanoparticles), or a combination of the two.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.