In silico study of reaction mechanisms and design principles for water oxidation catalysts

Leiden Repository

In silico study of reaction mechanisms and design principles for water oxidation catalysts

Title: In silico study of reaction mechanisms and design principles for water oxidation catalysts
Author: Vallés Pardo, José Luis
Publisher: Leiden Institute of Chemistry (LIC), Faculty of Science, Leiden Uni
Issue Date: 2012-12-19
Keywords: Ab-initio Molecular Dynamics
Homogeneous catalysis
Molecular modelling
Quantum Mechanics
Water oxidation catalysts
Abstract: Throughout the last decades the water oxidation process has been extensively investigated. However, open questions remain on the reaction mechanism and the possible intermediates in the catalytic cycle. Indeed, different catalysts can function through different reaction routes. Some of them work in a proton-coupled electron transfer (PCET) pathway, while other catalysts have a non-PCET behaviour. Some of these problems lie in the very short lifetime of intermediates, which makes it difficult to characterize them experimentally. Within this context, DFT calculations represent a very useful tool. In fact quantum-mechanical computational tools allow exploring and analyzing the possible intermediates and study and compare different reaction pathways in order to find the energetically most likely one. In the same way the thermodynamics of the catalytic cycle and the kinetics of the reaction coordinates can be analyzed. The specific aim of this thesis is the study of different catalysts and reaction pathways to find clues about the mechanism of the reaction and develop guiding principles for the design of efficient water oxidation complexes
Description: Promotor: Huub J.M. de Groot, Co-promotor: Francesco Buda
With summaries in Dutch, Catalan and Spanish
Faculty: Faculteit der Wiskunde en Natuurwetenschappen
Citation: Vallés Pardo, J.L., 2012, Doctoral thesis, Leiden University
Handle: http://hdl.handle.net/1887/20311
 

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application/pdf Chapter 1 Introduction 271.3Kb View/Open
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application/pdf Chapter 6 General discussion and outlook 104.1Kb View/Open
application/pdf Summary in Dutch 66.04Kb View/Open
application/pdf Summary 64.77Kb View/Open
application/pdf Summary in Catalan 65.15Kb View/Open
application/pdf Summary in Spanish 65.88Kb View/Open
application/pdf Curriculum Vitae_List of publications 63.27Kb View/Open
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