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The dynamic interplay between water and oxygen vacancy at the near-surface of ceria

Water, even at trace concentrations, strongly increases the CO oxidation activities of the reducible metal oxide supported noble-metal catalysts, where the transfer of proton plays a key role. In this paper, we performed a thorough investigation of the interplay between water molecules and the reduced CeO2(111) surface. It was found that water molecules can induce the migration of oxygen vacancies which in turn results in the formation of surface protons. The proton then entangles with the near-surface polaron to form polaron–proton pair due to their mutual attractive interactions. The hopping of the polaron can easily trigger the long-range or short-range diffusion of protons mediated by water molecules at the CeO2(111) surface. These findings provide new insights into the key roles of oxygen vacancies and polarons in reducible oxide based heterogeneous catalysis, which is beneficial for the understanding of the increased activity of reducible oxide supported metal nanoparticles in the presence of water.