Publication
Title
Accurate reaction probabilities for translational energies on both sides of the barrier of dissociative chemisorption on metal surfaces
Author
Abstract
Molecular dynamics simulations are essential for a better understanding of dissociative chemisorption on metal surfaces, which is often the rate-controlling step in heterogeneous and plasma catalysis. The workhorse quasi-classical trajectory approach ubiquitous in molecular dynamics is able to accurately predict reactivity only for high translational and low vibrational energies. In contrast, catalytically relevant conditions generally involve low translational and elevated vibrational energies. Existing quantum dynamics approaches are intractable or approximate as a result of the large number of degrees of freedom present in molecule-metal surface reactions. Here, we extend a ring polymer molecular dynamics approach to fully include, for the first time, the degrees of freedom of a moving metal surface. With this approach, experimental sticking probabilities for the dissociative chemisorption of methane on Pt(111) are reproduced for a large range of translational and vibrational energies by including nuclear quantum effects and employing full-dimensional simulations.
Language
English
Source (journal)
The journal of physical chemistry letters / American Chemical Society. - Washington, D.C, 2010, currens
Publication
Washington, D.C : American Chemical Society , 2024
ISSN
1948-7185
DOI
10.1021/ACS.JPCLETT.3C03408
Volume/pages
15 :9 (2024) , p. 2566-2572
ISI
001177959900001
Pubmed ID
38416779
Full text (Publisher's DOI)
Full text (open access)
UAntwerpen
Faculty/Department
Research group
Publication type
Subject
Affiliation
Publications with a UAntwerp address
External links
Web of Science
Record
Identifier
Creation 29.03.2024
Last edited 05.04.2024
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