CAREER:Hierarchical Modeling for Rational Catalyst Design in Aqueous Conditions

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Abstract (Getman, 1554385)The proposed research will refine molecular simulation models for catalytic reactions in the presence of liquid water and apply the calculations to an electrochemical process for ammonia synthesis that could potentially replace the long-standing, but energy intensive, Haber-Bosch gas phase process. The research is integrated with an educational plan that introduces molecular level simulation concepts to students across levels ranging from high school to graduate research.Theoretical understanding of catalytic materials and processes has advanced significantly in recent years due to rapid improvements in computer resources. This theoretical understanding is streamlining the process of catalyst discovery and moving the field of catalysis toward the prediction of new processes and materials and away from the traditional trial-and-error approach. However, this transition has been slow in the area of liquid phase catalysis, especially electrocatalysis, in large part because of incomplete understanding of the interactions that occur between fluid molecules and the catalyst surface. The research proposed here will take a large step toward better understanding these interactions by considering their free energies, whereas prior treatments have only considered their enthalpies. Traditional modeling equations will be refined and extended by adding, for the first time, free energy contributions due to rotation, translation, and interaction occurring between liquid-phase molecules and species adsorbed to the catalyst surface. The refined models will then be directed toward understanding the reaction between liquid water and gaseous nitrogen in an electrocatalytic environment to produce ammonia under near-ambient temperature and pressure conditions. The improved simulation models will pave the way for a more rational approach to catalyst discovery across a broad range of liquid phase catalytic reactions, and the educational materials will train coming generations of students in molecular-level phenomena and the effective use of molecular simulation tools.