Jump to main content
Jump to site search

Issue 25, 2014
Previous Article Next Article

Surface oxygen vacancies in gold based catalysts for CO oxidation

Author affiliations

Abstract

Experimental catalytic activity measurements, diffuse reflectance infrared Fourier spectroscopy, and density functional theory calculations are used to investigate the role and dynamics of surface oxygen vacancies in CO oxidation with O2 catalyzed by Au nanoparticles supported on a Y-doped TiO2 catalyst. Catalytic activity measurements show that the CO conversion is improved in a second cycle of reaction if the reactive flow is composed by CO and O2 (and inert) while if water is present in the flow, the catalyst shows a similar behaviour in two successive cycles. DRIFTS-MS studies indicate the occurrence of two simultaneous phenomena during the first cycle in dry conditions: the surface is dehydroxylated and a band at 2194 cm−1 increases (proportionally to the number of surface oxygen vacancies). Theoretical calculations were conducted in order to explain these observations. On one hand, the calculations show that there is a competition between gold nanoparticles and OH to occupy the surface oxygen vacancies and that the adsorption energy of gold on these sites increases as the surface is being dehydroxylated. On the other hand, these results evidence that a strong electronic transfer from the surface to the O2 molecule is produced after its adsorption on the Au/TiO2 perimeter interface (activation step), leaving the gold particle in a high oxidation state. This explains the appearance of a band at a wavenumber unusually high for the CO adsorbed on oxidized gold particles (2194 cm−1) when O2 is present in the reactive flow. These simultaneous phenomena indicate that a gold redispersion on the surface occurs under reactive flow in dry conditions generating small gold particles which are very active at low temperature. This fact is notably favoured by the presence of surface oxygen vacancies that improve the surface dynamics. The obtained results suggest that the reaction mechanism proceeds through the formation of a peroxo-like complex formed after the electronic transfer from the surface to the gas molecule.

Graphical abstract: Surface oxygen vacancies in gold based catalysts for CO oxidation

Back to tab navigation

Publication details

The article was received on 13 Nov 2013, accepted on 25 Feb 2014 and first published on 28 Feb 2014


Article type: Paper
DOI: 10.1039/C3RA46662K
Citation: RSC Adv., 2014,4, 13145-13152
  •   Request permissions

    Surface oxygen vacancies in gold based catalysts for CO oxidation

    F. Romero-Sarria, J. J. Plata, O. H. Laguna, A. M. Márquez, M. A. Centeno, J. F. Sanz and J. A. Odriozola, RSC Adv., 2014, 4, 13145
    DOI: 10.1039/C3RA46662K

Search articles by author

Spotlight

Advertisements