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Title: Theoretical studies in dye-sensitized solar cells and photo-catalysis at metal oxide interfaces
Author: Ip, Chung Man
ISNI:       0000 0004 6350 728X
Awarding Body: University of Warwick
Current Institution: University of Warwick
Date of Award: 2016
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In this thesis we present theoretical and computational studies for the p-type and n-type dye-sensitized solar cells (DSSCs), and the photo-catalytic reduction of carbon dioxide to generate methane. For p-type DSSCs, we computed the hole injection and recombination rate at the semiconductor-dye (NiO-C343) interface based on theories applied previously for electron injection and recombination in n-type DSSCs, derived from Fermi golden rule and non-adiabatic charge transfer theory. Our analysis showed that the faster recombination in p-type in comparison to n-type was due to difference in Franck-Condon factor of the relevant transitions. For n-type DSSCs, we devised a statistical model based on the electronic structural properties of dyes for predicting the efficiency of this device with confidence when a new dye was employed. The approach for constructing the model was QSAR-like and involved examining correlations between the efficiency of the device and a number of predictors that were properties of the dye. We also quantified the donor-π-acceptor (D-π-A) character of dyes and showed statistically that increasing the strength of this character was ineffective for improving the efficiency of n-type DSSCs. For photo-catalytic reduction of carbon dioxide to produce methane, we studied with DFT calculations three competing reaction mechanisms on TiO2 anatase(101) proposed in literature on the basis of experimentally observed reaction intermediates. By comparing the thermodynamics of mechanisms we showed that the formaldehyde pathway was the most favorable reaction mechanism. The computational methodology employed was useful for testing mechanistic hypotheses for reactions on the surface of solid catalysts.
Supervisor: Not available Sponsor: Engineering and Physical Sciences Research Council
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: QD Chemistry