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Title: Atmospheric Aerosol : The link between composition; and physical behaviour
Author: Corris, Benjamin Andrew
ISNI:       0000 0004 2679 9340
Awarding Body: The University of Manchester
Current Institution: University of Manchester
Date of Award: 2008
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The preparation and reactivity of a range of model systems for the low temperature oxidation of CO by gold catalysts have been investigated with a view to assessing their feasibility for bridging the 'materials gap' between well-defined single crystalline models and practical supported catalysts. The studied systems included gold powder, electrochemically oxidized gold foil, gold nanoparticles prepared on Ti02 single crystal surfaces by spin-coating and gold nanoparticles prepared on Ti02 powder by deposition-precipitation. Particular attention was paid to the reduction of oxidised gold species, since these are the common precursors in the preparation of practical nanoparticular catalysts. Oxidised gold species may also be mechanistically relevant for the catalytic low-temperature CO oxidation. A low volume reactor was designed for studies of flat gold model catalysts. It was tested with in situ X-ray absorption spectroscopy (XAS). The design of the reactor cell allows the use of further techniques including UVNis spectroscopy, X-ray differaction (XRD), Raman scattering and Infrared (IR) Spectroscopy. The reactor was also designed to permit reaction rate measurements with a mass spectrometer. In comparison to other reactors reported in the literature, this design is very cost efficient, not only in its construction but also due to its compatibility with a wide range of spectroscopic techniques. In situ X-ray photoelectron spectroscopy (XPS) on gold particles supported on Ti02 powder indicated that different atmosphere could change the morphology of the gold particles. This change is more prominent for smaller particles. The formation of graphite like spices under a CO atmosphere was observed as well. X-ray photoelectron spectroscopy (XPS) and in situ Au L-edge XAS indicated that suitable gold nanoparticles could be prepared by spin coating of tetrachloroauric acid solutions onto rutile single crystals. Gold loadings as low as 0.1 and 0.03 monolayers could be achieved. The XAS data indicated the presence of low average Au-Au coordination numbers, suggesting the presence of very small nanoparticles. XA spectra taken under CO and O2atmosphere indicated that CO interacts with the gold particles.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available