Water-Related Adsorbates on Stepped Platinum Surfaces

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Water-Related Adsorbates on Stepped Platinum Surfaces

Type: Doctoral Thesis
Title: Water-Related Adsorbates on Stepped Platinum Surfaces
Author: Kolb, Manuel Jerome
Publisher: Department of Catalysis and Surface Chemistry, Leiden Institute of Chemistry (LIC), Faculty of Science, Leiden University
Issue Date: 2016-03-23
Keywords: DFT
Water
Adsorption
Solvation
Electrochemistry
Abstract: In this study we focused on the simulation of the interaction of water and its dissociation products hydrogen, oxygen and OH with platinum surfaces that contain a periodic arrangement of single-atom-high steps. We simulate these interactions using the framework of density functional theory and employ high-performance computing resources such as the Cartesius supercomputer of SURFsara. We find that the two possible types of step edges exhibit increased binding strengths compared to the flat parts of the interface. This binding strength is a key factor in the chemical reactivity of these surfaces. Furthermore, we investigate the structure of higher coverages of water molecules around the step edges, where we observe surprising changes, namely the appearance of four, five and seven-membered rings, compared to the six-membered rings that are usually observed on the flat surfaces. Our predictions for these structures are confirmed using high-resolution scanning tunneling microscopy data. Our results are among the first simulations of high-coverage water adsorption on regularly stepped platinum surfaces, which will help advance our understanding of solvation effects at the step edges, which are relevant for the fields of solvation science, electrochemistry and surface science.
Description: Promotor: M.T.M. Koper, Co-Promotor: L.B.F. Juurlink
Faculty: Faculteit der Wiskunde en Natuurwetenschappen
Citation: Kolb, M.J., 2016, Doctoral Thesis, Leiden University
ISBN: 9789402800937
Handle: http://hdl.handle.net/1887/38619
 

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