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O: Fachverband Oberflächenphysik
O 67: Symposium: The Solid-Liquid Interface: A Challenge for Theoreticians II
O 67.2: Hauptvortrag
Freitag, 30. März 2007, 10:45–11:15, H38
Modeling the Electrochemical Potential of the Aqueous-Electrode Interface within Periodic Density Functional Theory — •Sally Wasileski1, Christopher Taylor2, Michael Janik2, and Matthew Neurock2 — 1Department of Chemistry, University of North Carolina at Asheville, Asheville, NC 28804 USA — 2Departments of Chemical Engineering and Chemistry, University of Virginia, Charlottesville, VA 22904 USA
Ab-initio methods such as density functional theory (DFT), used extensively in modeling the structure and reactivity of adsorbates at vacuum interfaces, are now capable of probing energies and pathways for complex metal/solution environments and are proving to be a good complement to experimental efforts. A model has been developed to include the influence of the tunable electrochemical potential at the aqueous-electrode interface within the periodic density functional theory methodology [Taylor, CD, Wasileski, SA, Filhol, J-S, Neurock, M, "First principles reaction modeling of the electrochemical interface: Consideration and calculation of a tunable surface potential from atomic and electronic structure" Phys. Rev. B (2006) 73, 165402/1-165402/16]. Specific aspects of the model will be addressed in detail along with examples of using the methodology to investigate electrocatalytic reactions such as potential-dependent water dissociation at VIII and IB surfaces and potential-dependent methanol dehydrogenation and carbon monoxide oxidation (relevant chemistry to direct methanol fuel cells).