“…Surface science studies of model systems for oxides, particularly well-defined oxide thin films, have been proven to be an effective approach. − The effect of F centers on the physical chemistry and reactivity of MgO surface has been comprehensively investigated and understood employing MgO(001) thin films as model systems. − The influence of oxygen vacancies on the physical chemistry and reactivity of reducible oxides such as TiO 2 and CeO 2 has also been extensively studied employing corresponding oxide single crystals and single crystal thin films. − F centers and oxygen vacancies on oxide surfaces are easily hydroxylated to form surface hydroxyls. Depending on the nature of metal oxides, surface hydroxyls can serve either as the Brönsted acid sites or as the Brönsted base sites, can result in the delocalization of electrons at metal oxide surfaces, , can drive the surface reconstruction of metal oxide surfaces, − and can affect the dispersion and aggregation of the supported metal component. − Surface hydroxyls on metal oxides exclusively in the form of H bonded to surface lattice oxygen anion (herein defined as lattice surface hydroxyls) are also key surface intermediates in several important heterogeneous catalytic reactions including H 2 oxidation, methanol synthesis, dehydrogenation reaction, water gas shift reaction (WGS), and preferential oxidation of CO in H 2 (PROX). − Therefore, it is of great importance to fundamentally understand the reactivity of lattice surface hydroxyls on metal oxides. The reactivity of hydroxyls on RuO 2 (110)/Ru(0001) − and ZnO(101̅0) − model surfaces have been quite well understood.…”