Allan, Michael James; (2020) Crystallography and Electronic Structure of Model Metal Oxide Catalysts. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

This thesis embodies work studying multiple hydrogen producing metal oxide catalysts as both single crystals alongside ultra-thin films. The first catalyst study investigates the water splitting properties of titanium dioxide by scanning tunnelling microscopy. By exploring the excess electron distribution around hydroxyls upon water splitting at an oxygen vacancy, mechanistic details from the process, along with electronic properties of the surface have been resolved. The second catalyst explored is cerium dioxide ultra-thin films and studying both their oxidised and reduced states. As ceria is involved in the water-gas shift reaction, an important reaction which oxidises carbon monoxide with water to produce hydrogen and carbon dioxide, the understanding of its surface and any reconstructions is of great significance. This is studied by scanning tunnelling microscopy to understand the differences of the films, and high-resolution electron energy loss spectroscopy (HREELS) to give insight into the bonding environments that give rise to reconstructions. The third catalyst studied is ceria-zirconia mixed metal oxide. The addition of zirconia to ceria improves its performance in the water-gas shift reaction. By studying the redox behaviour of the catalyst in the form of an inverse model catalyst by LEED, XPEEM, XAS and XPS, the synergy understanding between both metals has been furthered.

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