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First-Principles Analysis of the Stability of Water on the Oxidised and Reduced CuO(111) Surface

preprint
submitted on 27.10.2017 and posted on 30.10.2017 by Marco Fronzi, Michael Nolan
We use fi rst-principles Density Functional Theory calculations with inclusion of the Hubbard +U correction (DFT+U) on the Cu 3d states, to investigate the interaction of water with the 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 energetics, geometry and electronic structure of relevant confi gurations 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 signi ficant 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.

Funding

SFI US/14/E2915

History

Topic

  • Catalysts
  • Materials Processing

Email Address of Submitting Author

michael.nolan@tyndall.ie

Email Address(es) for Other Author(s)

marco.fronzi@xjtu.edu.cn

Institution

Xi'an Jiaotong University and Tyndall National Institute

Country

China and Ireland

ORCID For Submitting Author

0000-0002-5224-8580

Declaration of Conflict of Interest

No conflict of Interest

Exports