Water-Related Adsorbates on Stepped Platinum Surfaces

Leiden Repository

Water-Related Adsorbates on Stepped Platinum Surfaces

Type: Doctoral Thesis
Title: Water-Related Adsorbates on Stepped Platinum Surfaces
Author: KolbManuel, Jerome
Issue Date: 2016-03-23
Keywords: 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.
Promotor: Supervisor: M.T.M. Koper Co-Supervisor: L.B.F. Juurlink
Faculty: Faculty of Science
University: Leiden University
Uri: urn:isbn:9789402800937
Handle: http://hdl.handle.net/1887/38619

Files in this item

Description Size View
application/pdf Full Text 23.66Mb View/Open
application/pdf Cover 305.9Kb View/Open
application/pdf Title Pages_Contents 196.0Kb View/Open
application/pdf Chapter 1 1.337Mb View/Open
application/pdf Chapter 2 3.045Mb View/Open Full text at publisher site
application/pdf Chapter 3 2.423Mb View/Open Full text at publisher site
application/pdf Chapter 4 9.556Mb View/Open
application/pdf Chapter 5 8.226Mb View/Open
application/pdf Chapter 6 147.7Kb View/Open
application/pdf Chapter 7 138.2Kb View/Open
application/pdf Chapter 8 135.3Kb View/Open
application/pdf Publications_Curriculum Vitae 165.5Kb View/Open
application/pdf Propositions 72.63Kb View/Open

This item appears in the following Collection(s)