Regensburg 2022 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 31: Solid-Liquid Interfaces 3: Reactions and Electrochemistry
O 31.5: Vortrag
Dienstag, 6. September 2022, 11:45–12:00, S054
Modeling varying potential conditions in electrochemical simulations: The case of O2/Au(111) — •Elias Diesen, Alexandra M. Dudzinski, Hendrik H. Heenen, Vanessa J. Bukas, and Karsten Reuter — Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin
While significant insight has been gained in recent years by DFT-based simulations of electrochemical processes, crucial methodological challenges remain, especially for accurate determination of reaction energies under operando conditions. One open question is how to represent the constant electrode potential in simulations of an electrified water/metal interface, where the simulation setup requires a constant charge in the simulation cell throughout the reaction. Here we compare different levels of treatment of the electrochemical interface: explicit ab initio molecular dynamics, an implicit solvent model, and a sawtooth-potential electric field in vacuum, for the case of O2 adsorption on Au(111). We characterize the dynamics near the surface and identify ways an applied electrode potential influences the adsorption. We find, in all methods, significantly enhanced O2 adsorption at more reducing conditions. However, we also show that certain aspects of the process can only be captured using a fully explicit treatment of the solvent.