First-principles analysis of the stability of water on oxidised and reduced CuO(111) surfaces
| Autor: | Marco Fronzi, Michael Nolan |
|---|---|
| Rok vydání: | 2017 |
| Předmět: |
Water adsorption
Materials science General Chemical Engineering Ab initio Thermodynamics Oxygen vacancy stabilization 02 engineering and technology General Chemistry Electronic structure 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Dissociation (chemistry) 0104 chemical sciences symbols.namesake Copper oxides Adsorption Vacancy defect Desorption Density functional theory symbols van der Waals force 0210 nano-technology Oxygen vacancy sites |
| Zdroj: | RSC Advances. 7:56721-56731 |
| ISSN: | 2046-2069 |
| DOI: | 10.1039/c7ra11854f |
| Popis: | © 2017 The Royal Society of Chemistry. We use first-principles density functional theory calculations including the Hubbard + U correction (PBE + U) on Cu-3d states to investigate the interaction of water with a CuO(111) surface. We compute adsorption energies and the stability of different water coverages, with a particular focus on the interaction of water with oxygen vacancy sites, and how vacancy stabilization occurs. We study the energetics, geometry and electronic structure of relevant configurations, finding that there are only small changes to the local geometry around the water adsorption site(s) and the electronic properties. The inclusion of van der Waals interactions has no significant impact on the stability of water on CuO(111). We extend the analysis to include realistic environmental conditions within the ab initio atomistic thermodynamics framework, which allows us to assess the stability of the water/copper-oxide system as a function of ambient conditions, and focus on three important surface processes: water adsorption/desorption on the stoichiometric surface, conditions for dissociation, and oxygen vacancy stabilization. |
| Databáze: | OpenAIRE |
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