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A combined molecular dynamics+quantum mechanics method for investigation of dynamic effects on local surface structures
Uppsala University, Teknisk-naturvetenskapliga vetenskapsområdet, Chemistry, Department of Materials Chemistry.
2004 In: Journal of Chemical Physics, ISSN 0021-9606, Vol. 120, no 10, 4939-4948 p.Article in journal (Refereed) Published
Place, publisher, year, edition, pages
2004. Vol. 120, no 10, 4939-4948 p.
Identifiers
URN: urn:nbn:se:uu:diva-93852OAI: oai:DiVA.org:uu-93852DiVA: diva2:167470
Available from: 2005-12-23 Created: 2005-12-23Bibliographically approved
In thesis
1. Combined Molecular Dynamics and Embedded-Cluster Calculations in Metal Oxide Surface Chemistry
Open this publication in new window or tab >>Combined Molecular Dynamics and Embedded-Cluster Calculations in Metal Oxide Surface Chemistry
2005 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The development and improvement of the functionality of metal oxides in heterogeneous catalysis and other surface chemical processes can greatly benefit from an atomic-level understanding of the surface chemistry. Atomistic calculations such as quantum mechanical (QM) calculations and molecular dynamics (MD) simulations can provide highly detailed information about the atomic and electronic structure, and constitute valuable complements to experimental surface science techniques.

In this thesis, an embedded-cluster approach for quantum mechanical calculations has been developed to model the surface chemistry of metal oxides. In particular, CO adsorption on the MgO(001) and CeO2(110) surfaces as well as O vacancy formation at the CeO2(110) surface have been investigated. The cluster model has been thoroughly tested by comparison with electronic structure calculations for the periodic slab model.

The chemical implications of distorted surface structures arising from the surface dynamics have been investigated by combining the QM embedded-cluster calculations with force-field based MD simulations. Here QM embedded-cluster calculations were performed using surface structures sampled from the MD simulations.

This combined MD+QM embedded-cluster procedure was applied to the CO adsorption on MgO(001) at 50 K and the O vacancy formation on CeO2(110) at 300 K. Significant thermal variations of the CO adsorption energy and the O vacancy formation energy were observed. It was found that these variations could be estimated using the force field of the MD simulation as an interaction model. With this approach, the QM results were extrapolated to higher temperature and doped systems.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2005. 52 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 130
Keyword
Inorganic chemistry, embedded-cluster, ab initio, molecular dynamics, metal oxide, ceria, magnesium oxide, adsorption, surface defect, Oorganisk kemi
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-6227 (URN)91-554-6422-X (ISBN)
Public defence
2006-01-19, Room 2001, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15
Opponent
Supervisors
Available from: 2005-12-23 Created: 2005-12-23 Last updated: 2013-09-18Bibliographically approved

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