Energy conversion dynamics of chemical processes at surfaces from first principles

Samenvatting

Chemical reactions go hand-in-hand with an energy exchange with the environment in which they take place. Surfaces offer a variety of energy dissipation channels, constituted by the nuclear and electronic degrees of freedom of the surface atoms. An atomic scale understanding of the energy exchange during chemical reaction dynamics is however only very limited at best - despite important implications for example for heterogeneous as well as electrocatalysis and astrochemistry. In order to accurately account for bond breaking and making, first-principles based modelling is required. It finds itself challenged by the necessity to deal with a huge number of atoms in order to describe environmental heat baths. In case of electrochemistry, solvation and electrolyte effects are inherently long-ranged, dynamical and nonlinear.
I propose to employ and further develop embedding techniques to face this challenge, in particular a recently proposed novel embedding scheme for metallic systems (QM/Me, Meyer and Reuter, Angew. Chem. Int. Ed. 53, (2014) 4721). Comparison with time-resolved x-ray photoelectron spectroscopy measurements for reaction dynamics of O2 on Pt(111) measured by my collaborator G. Mercurio at the free electron laser in Hamburg (FLASH) will allow to scrutinize the embedding model. An extension to the electrochemical CO2 reduction on Cu(111) will be based on a recently developed charge-optimized many-body force field (Sinnott et al., Cat. Comm. 52, (2014) 84) in order to include the solvent in the embedding. Finally, modeling energy exchange during chemical reactions on dust grains in the interstellar medium with embedding broadens the scope of the technique and promises to offer novel insights for astrochemistry.

Producten

Wetenschappelijk artikel

Kenmerken

Projectnummer

723.014.009

Hoofdaanvrager

Dr. J. Meyer

Verbonden aan

Universiteit Leiden, Faculteit der Wiskunde en Natuurwetenschappen, Leiden Institute of Chemistry

Uitvoerders

M.J. Kolb MSc, Dr. J. Meyer, Drs. F. Nattino, N.B. Niet Bekend en Niet Gebruiken, S Rasti MSc, S. Seal MSc

Looptijd

01/11/2015 tot 13/11/2019