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Title: When ruthenia met titania: Achieving extraordinary catalytic activity at low temperature by nanostructuring of oxides

Abstract

Nanostructured RuOx/TiO2(110) catalysts have a remarkable catalytic activity for CO oxidation at temperatures in the range of 350–375 K. Furthermore, the RuO2(110) surface has no activity. The state-of-the-art DFT calculations indicate that the main reasons for such an impressive improvement in the catalytic activity are: (i) a decrease of the diffusion barrier of adsorbed O atoms by around 40%, from 1.07 eV in RuO2(110) to 0.66 eV in RuOx/TiO2(110), which explains the shift of the activity to lower temperatures and (ii) a lowering of the barrier by 20% for the association of adsorbed CO and O species to give CO2 (the main barrier for the CO oxidation reaction) passing from around 0.7 eV in RuO2(110) to 0.55 eV in RuOx/TiO2(110). We show that the catalytic properties of ruthenia are strongly modified when supported as nanostructures on titania, attaining higher activity at temperatures 100 K lower than that needed for pure ruthenia. As in other systems consisting of ceria nanostructures supported on titania, nanostructured ruthenia shows strongly modified properties compared to the pure oxide, consolidating the fact that the nanostructuring of oxides is a main way to attain higher catalytic activity at lower temperatures.

Authors:
 [1];  [2];  [2];  [3];  [4];  [2];  [1]
  1. Univ. de Sevilla, Sevilla (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. Central de Venezuela, Caracas (Venezuela)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States); Instituto Venezolano de Investigaciones Cientificas (IVIC), Caracas (Venezuela)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1234376
Report Number(s):
BNL-111670-2015-JA
Journal ID: ISSN 1463-9076; PPCPFQ; R&D Project: CO009; KC0302010
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 17; Journal Issue: 40; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Graciani, J., Stacchiola, D., Yang, F., Evans, J., Vidal, A. B., Rodriguez, J. A., and Sanz, J. F. When ruthenia met titania: Achieving extraordinary catalytic activity at low temperature by nanostructuring of oxides. United States: N. p., 2015. Web. doi:10.1039/c5cp04638f.
Graciani, J., Stacchiola, D., Yang, F., Evans, J., Vidal, A. B., Rodriguez, J. A., & Sanz, J. F. When ruthenia met titania: Achieving extraordinary catalytic activity at low temperature by nanostructuring of oxides. United States. https://doi.org/10.1039/c5cp04638f
Graciani, J., Stacchiola, D., Yang, F., Evans, J., Vidal, A. B., Rodriguez, J. A., and Sanz, J. F. Wed . "When ruthenia met titania: Achieving extraordinary catalytic activity at low temperature by nanostructuring of oxides". United States. https://doi.org/10.1039/c5cp04638f. https://www.osti.gov/servlets/purl/1234376.
@article{osti_1234376,
title = {When ruthenia met titania: Achieving extraordinary catalytic activity at low temperature by nanostructuring of oxides},
author = {Graciani, J. and Stacchiola, D. and Yang, F. and Evans, J. and Vidal, A. B. and Rodriguez, J. A. and Sanz, J. F.},
abstractNote = {Nanostructured RuOx/TiO2(110) catalysts have a remarkable catalytic activity for CO oxidation at temperatures in the range of 350–375 K. Furthermore, the RuO2(110) surface has no activity. The state-of-the-art DFT calculations indicate that the main reasons for such an impressive improvement in the catalytic activity are: (i) a decrease of the diffusion barrier of adsorbed O atoms by around 40%, from 1.07 eV in RuO2(110) to 0.66 eV in RuOx/TiO2(110), which explains the shift of the activity to lower temperatures and (ii) a lowering of the barrier by 20% for the association of adsorbed CO and O species to give CO2 (the main barrier for the CO oxidation reaction) passing from around 0.7 eV in RuO2(110) to 0.55 eV in RuOx/TiO2(110). We show that the catalytic properties of ruthenia are strongly modified when supported as nanostructures on titania, attaining higher activity at temperatures 100 K lower than that needed for pure ruthenia. As in other systems consisting of ceria nanostructures supported on titania, nanostructured ruthenia shows strongly modified properties compared to the pure oxide, consolidating the fact that the nanostructuring of oxides is a main way to attain higher catalytic activity at lower temperatures.},
doi = {10.1039/c5cp04638f},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 40,
volume = 17,
place = {United States},
year = {Wed Sep 09 00:00:00 EDT 2015},
month = {Wed Sep 09 00:00:00 EDT 2015}
}

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