CAREER:Revolutionizing Propylene Production via Oxidative Dehydrogenation and CO2 Dissociation in Tandem

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The development of catalytic routes for converting lower alkanes to olefins is a challenging problem with high potential payoff due to the vast shale gas resources that have recently become available. The overarching goal of this project is to revolutionize propylene production from alkanes through an innovative tandem catalytic reaction scheme that improves overall conversion and selectivity. The project is based on a potentially transformative approach where new paradigms in reaction mechanisms guide catalyst synthesis. A hierarchical framework will be developed for rational design and characterization of catalysts with significant potential broader impact in the energy, petrochemical and chemical sectors of the US industry.The main objective of this project is to develop a new class of bifunctional catalysts based on sub-stoichiometric nanophase metal oxides that will work in a tandem reaction scheme, where oxidative dehydrogenation of alkanes and carbon dioxide reduction, via dissociative adsorption, will occur simultaneously without producing syngas. The proposed novel tandem reaction scheme has the potential to intensify on-purpose propylene production by preventing side reactions, such as coke formation, and further aromatization of propylene. A new facile synthesis method for producing oxygen-deficient anatase nanosheet catalysts is proposed by utilizing highly amorphous solubilized cellulose as a sacrificial template. The proposed experimental framework is based on optical reactor prototyping and Operando spectroscopy, where the molecular structure and reactivity of the metal oxide catalysts are studied simultaneously in a single optical cell by time- and spatially-resolved Raman spectroscopy under real working conditions. Integration of research and education is focused towards modernizing the chemical reaction engineering curriculum with teaching modules on Operando spectroscopy. Outreach efforts are aimed at engaging K-12 students, including underrepresented minorities, by developing a freeware computer game that teaches principles of molecular symmetry and spectroscopy.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.