First Principles Studies of Water and Ice on
Department of Chemistry
University College London
Thesis submitted for the degree of Doctor of Philosophy
I, Xiaoliang Hu, confirm that the work presented in this thesis is my own. Where in-
formation has been derived from other sources, I confirm that this has been indicated
in the thesis.
The interaction of water (and ice) with oxide surfaces has been studied with first prin-
ciples density functional theory. To begin, an extensive series of studies on the clay
mineral kaolinite (Al2Si2O5(OH)4) are reported with a view to understanding the effi-
cacy of kaolinite as a heterogeneous ice nucleating agent. The main conclusions are:
(i) water clustering is disfavoured on the kaolinite surface; (ii) a stable two dimensional
ice-like water overlayer can form; (iii) water covered kaolinite is itself "hydrophobic"
compared to the bare "hydrophilic" kaolinite surface; and (iv) it is shown that ampho-
terism (the ability to accept and donate H bonds) of the hydroxylated kaolinite surface