The reactivity of zirconia nanoparticles has been investigated by means of DFT+U calculations as a function of the morphology and stoichiometry. For comparative purposes, a single Au atom has been deposited on the stoichiometric and O-deficient regular (101) surface, on the stepped (156) surface, and on nanoparticles in the range of 0.9-1.9 nm in size. We show that, under stoichiometric conditions, nanostructuring leads to enhanced binding energies and redox processes with the supported metal that are not found on the extended surfaces. These new features are due to the structural flexibility and peculiar electronic structure displayed by the nanoparticles. In this respect, nanostructuring of oxide supports can modify and possibly improve the catalytic activity of the deposited metals. In contrast, we show that under reducing conditions nanostructuring stabilizes the O vacancies making zirconia nanoparticles less reactive toward Au adsorption than O-deficient extended surfaces.

RUIZ PUIGDOLLERS, A., Illas, F., Pacchioni, G. (2016). Effect of Nanostructuring on the Reactivity of Zirconia: A DFT+U Study of Au Atom Adsorption. JOURNAL OF PHYSICAL CHEMISTRY. C, 120(31), 17604-17612 [10.1021/acs.jpcc.6b05685].

Effect of Nanostructuring on the Reactivity of Zirconia: A DFT+U Study of Au Atom Adsorption

RUIZ PUIGDOLLERS, ANTONIO
Primo
;
PACCHIONI, GIANFRANCO
2016

Abstract

The reactivity of zirconia nanoparticles has been investigated by means of DFT+U calculations as a function of the morphology and stoichiometry. For comparative purposes, a single Au atom has been deposited on the stoichiometric and O-deficient regular (101) surface, on the stepped (156) surface, and on nanoparticles in the range of 0.9-1.9 nm in size. We show that, under stoichiometric conditions, nanostructuring leads to enhanced binding energies and redox processes with the supported metal that are not found on the extended surfaces. These new features are due to the structural flexibility and peculiar electronic structure displayed by the nanoparticles. In this respect, nanostructuring of oxide supports can modify and possibly improve the catalytic activity of the deposited metals. In contrast, we show that under reducing conditions nanostructuring stabilizes the O vacancies making zirconia nanoparticles less reactive toward Au adsorption than O-deficient extended surfaces.
Articolo in rivista - Articolo scientifico
Physical and Theoretical Chemistry; Electronic, Optical and Magnetic Materials; Surfaces, Coatings and Films; Energy (all)
English
17604
17612
9
RUIZ PUIGDOLLERS, A., Illas, F., Pacchioni, G. (2016). Effect of Nanostructuring on the Reactivity of Zirconia: A DFT+U Study of Au Atom Adsorption. JOURNAL OF PHYSICAL CHEMISTRY. C, 120(31), 17604-17612 [10.1021/acs.jpcc.6b05685].
RUIZ PUIGDOLLERS, A; Illas, F; Pacchioni, G
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/10281/132201
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