RT info:eu-repo/semantics/article
T1 The oxygen evolution reaction at MoS2 edge sites: The role of a solvent environment in DFT-based molecular simulations
A1 German Gorosito, Estefanía
A1 Gebauer, Ralph
K1 Oxygen evolution reaction
K1 Water - Electrolysis
K1 Electrólisis
K1 Density functionals
K1 Mathematical physics
K1 Física matématica
K1 Molybdenum disulfide
K1 Analytical chemistry
K1 22 Física
K1 2301 Química Analítica
AB Density functional theory (DFT) calculations are employed to study the oxygen evolution reaction (OER) on the edges of stripes of monolayer molybdenum disulfide. Experimentally, this material has been shown to evolve oxygen, albeit with low efficiency. Previous DFT studies have traced this low catalytic performance to the unfavourable adsorption energies of some reaction intermediates on the MoS2 edge sites. In this work, we study the effects of the aqueous liquid surrounding the active sites. A computational approach is used, where the solvent is modeled as a continuous medium providing a dielectric embedding of the catalyst and the reaction intermediates. A description at this level of theory can have a profound impact on the studied reactions: the calculated overpotential for the OER is lowered from 1.15 eV to 0.77 eV. It is shown that such variations in the reaction energetics are linked to the polar nature of the adsorbed intermediates, which leads to changes in the calculated electronic charge density when surrounded by water. These results underline the necessity to computationally account for solvation effects, especially in aqueous environments and when highly polar intermediates are present.
PB MDPI
SN 1420-3049
YR 2023
FD 2023
LK https://uvadoc.uva.es/handle/10324/66517
UL https://uvadoc.uva.es/handle/10324/66517
LA eng
NO Molecules, 2023, Vol. 28, Nº. 13, 5182
NO Producción Científica
DS UVaDOC
RD 03-jun-2024