Reducibility of ZrO2 /Pt3 Zr and ZrO2 /Pt 2D films compared to bulk zirconia: a DFT+U study of oxygen removal and H2 adsorption

Nanoscale
Antonio Ruiz Puigdollers, Gianfranco Pacchioni

Abstract

Oxide reducibility is an important property that determines the chemical and physical behavior of the materials under working conditions. Zirconia is a non-reducible oxide that exhibits high resistance to the loss of oxygen and low reactivity towards hydrogen, two typical processes involved in oxide reduction. Oxide reducibility can change substantially by nanostructuring (e.g. formation of nanoparticles). In this study, we investigate theoretically by means of DFT+U calculations including dispersion interactions the properties of 2D zirconia films supported on a Pt3Zr alloy and Pt metal surfaces, two systems recently prepared experimentally. The results show that the supported ZrO2 ultrathin films behave very differently from the corresponding bulk oxide, with a low formation energy of oxygen vacancies, and a clear tendency to split the H2 molecule homolytically with direct reduction of the oxide. The comparison of free-standing and supported ZrO2 films shows that these peculiar properties are not due to the formation of a 2D nanostructure, but rather to the presence of the metal support and of a metal/oxide interface. The results provide evidence for the uncommon properties of supported 2D oxides.

References

Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Jul 15, 1991·Physical Review. B, Condensed Matter·V I AnisimovO K Andersen
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Jun 6, 2003·Nature·Chris G Van de Walle, J Neugebauer
Nov 2, 2004·Nature Materials·Stuart S P ParkinSee-Hun Yang
Sep 7, 2006·Journal of Computational Chemistry·Stefan Grimme
Dec 13, 2006·Physical Review Letters·Cristiana Di ValentinAnnabella Selloni
Sep 27, 2008·Chemical Society Reviews·Hans-Joachim Freund, Gianfranco Pacchioni
Oct 5, 2010·Physical Chemistry Chemical Physics : PCCP·Sergio Tosoni, Joachim Sauer
Aug 3, 2011·Accounts of Chemical Research·Livia Giordano, Gianfranco Pacchioni
Aug 1, 2012·Chemistry : a European Journal·Gianfranco Pacchioni
Feb 14, 2015·Nanoscale·Sergey M KozlovStefan T Bromley
Jun 7, 2016·Scientific Reports·Apurba SinhamahapatraJong-Sung Yu
Aug 18, 2016·Journal of the American Chemical Society·Md Anisur RahmanKam Tong Leung

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Citations

Apr 27, 2018·Chemical Society Reviews·Gianfranco Pacchioni, Hans-Joachim Freund
Jan 17, 2019·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Ho Viet ThangGianfranco Pacchioni

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