As the oxygen chemical potential decreases, the stoichiometric TiO2 surface undergoes reduction to TiO1.98, starting at ∆𝜇 O < -4 eV, by the loss of one two-fold (2f) bridging oxygen ). This creates an oxygen vacancy (VO) at the site and two five-fold titanium (Ti 5f ) atoms at the surface. The stability, electronic structures, and catalytic significance of this mildly reduced structure have been thoroughly explored in the literature . Notably, on the TiO2(110) surface, which acts as a reducible support for metal cluster catalysts, the surface VO plays a crucial role in enhancing catalytic activity by providing reactive sites that promote the adsorption and growth of catalytic metal clusters . These vacancies enhance reactions like CO oxidation, hydrogen production, and CO2 activation by increasing the reactivity and modifying the electronic properties of the metal clusters.