Sharon Hammes-Schiffer: Proton-Coupled Electron Transfer in Catalysis and Energy Conversion
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Event Date: 
Mon, 03/19/2012 - 4:00pm
Chemistry Building, Carolyn Hoff Lynch Room

Sharon Hammes-Schiffer
Department of Chemistry, Pennsylvania State University, University Park, PA  16802

Proton-coupled electron transfer (PCET) reactions play a vital role in a wide range of biological and chemical processes.  This talk will focus on recent advances in the theory of PCET.  The quantum mechanical effects of the active electrons and transferring proton, as well as the motions of the proton donor-acceptor mode and solvent or protein environment, are included in a general theoretical formulation.  This approach enables the calculation of rates and kinetic isotope effects, as well as the temperature and pH dependence, for comparison to experiment.  Applications to PCET reactions in solution, enzymes, and electrochemical systems will be presented.  These theoretical studies assist in the interpretation of experimental data and provide experimentally testable predictions.  In addition, recent developments of theoretical approaches for simulating the ultrafast dynamics of photoinduced PCET will be discussed.  Applications of these approaches to model systems illustrate both sequential and concerted mechanisms, as well as more complex branching processes involving a combination of sequential and concerted mechanisms.  These calculations also provide insights into the roles of proton vibrational relaxation and nonequilibrium solvent dynamics in photoinduced PCET processes and provide an explanation for experimentally observed deuterium isotope effects.

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