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Density functional theory study of trends in water dissociation on oxygen-preadsorbed and pure transition metal surfaces

Mario Mäkinen, Kari Laasonen

2023Surface Science20 citationsDOIOpen Access PDF

Abstract

Oxygen and water are the most reactive gases of the ambient air. The adsorption of both molecules on transition metal surfaces have been studied extensively, but mostly separately. However, water and oxygen usually co-exist, and therefore realistic systems need to take into consideration both simultaneously. As these adsorption reactions are so common, state-of-the-art results are beneficial as they capture large trends as accurately as possible. A comprehensive study of oxygen and water co-adsorption and dissociation on Ag(111)-, Au(111)-, Pd(111)-, Pt(111)-, Rh(111)- and Ni(111)-surfaces have been performed using density functional theory. We present a very strong general trend, where dissociated oxygen systematically lowers the activation energy of water dissociation on transition metal surfaces. This makes the oxygen dissociation the rate-determining step of the water dissociation reaction. The effect is caused by the additional pathway that the dissociated oxygen enables for the dissociation of water molecule.

Topics & Concepts

Dissociation (chemistry)OxygenAdsorptionChemistrySelf-ionization of waterDensity functional theoryTransition metalMoleculeMetalActivation energyPhotochemistryChemical physicsInorganic chemistryCatalysisPhysical chemistryComputational chemistryOrganic chemistryCatalytic Processes in Materials ScienceAdvanced Chemical Physics Studiesnanoparticles nucleation surface interactions