CAREER: Molecular Engineering of Catalytic Surface Chemistry Through First-Principles Simulation

点击翻译按钮获取中文摘要

ABSTRACT Proposal Title: Molecular Engineering of Catalytic Surface Chemistry Through First-Principles Simulation Proposal Number: CTS-9702762 Principal Investigator: Matthew Neurock Institution: University of Virginia, Charlottesville Density functional theory (DFT), transition state theory (TST), and Monte Carlo simulation (MC), are combined to study the mechanism of chemical reactions on metal surfaces. In particular, this proposal is focused on the synthesis of vinyl acetate on Au-promoted Pd catalyst. The reaction is of relevance in the plastics industry. Some fundamental issues, such as the effects of surface structure and adsorbed oxygen, are not completely understood. This selective oxidation chemistry is analyzed in terms of metal cluster structure and composition, adsorbate bonding, oxygen coverage and possible pathways. Energetics of adsorption and energy barriers of intermediate formation are calculated with DFT, intrinsic kinetics of the many possible steps are computed from TST, and macroscopic kinetics are calculated from MC simulations. The experimental validation of energetics and kinetics involves temperature-programmed desorption at UHV and reaction both at UHV and ambient pressure conditions, in work to be carried out by collaborators at DuPont. At the educational level, the PI will strengthen the chemical engineering curriculum in the area of computational chemistry. Two new courses in computational chemistry for undergraduate and graduate students and a course in molecular modeling for industry will be developed.