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Title: Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO2 catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures

Abstract

The ability of Au/TiO2 catalysts to promote the oxidation of carbon monoxide at cryogenic temperatures was probed by using diffuse-reflectance infrared absorption spectroscopy (DRIFTS). The aim of this work was to identify correlations between the catalytic activity and both the nature of the titania support and the size of the Au nanoparticles (NPs). Two key intermediates were identified: an initial CO adsorbed on defect sites within the titania support with a 2175 cm-1 C–O stretching frequency signature, and a second species with a DRIFTS peak at 2163 cm-1 associated with the intermediate at Au–TiO2 interfacial sites that incorporates atomic oxygen to produce CO2. CO adsorption at the low temperatures associated with this process (120 K) appears to require defective sites, possibly titanate-type surface species: an amorphous (and NaOH-treated) support showed higher activity than crystalline titania. Furthermore, the catalytic activity peaks at an Au NP average size of about 3 nm, which, in turn, correlates with the population of the second CO intermediate mentioned above. The mechanism that explains this cryogenic oxidation reaction is different than that extensively reported for the room-temperature processes, but both appear to display similar dependence on Au NP diameter.

Authors:
 [1]; ORCiD logo [1]
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  1. Univ. of California, Riverside, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Riverside, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1593411
Alternate Identifier(s):
OSTI ID: 1545965
Grant/Contract Number:  
SC0001839; FG02-09ER16096; FG02-03ER46599; FG02- 09ER16096
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 5; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lee, Ilkeun, and Zaera, Francisco. Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO2 catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures. United States: N. p., 2019. Web. doi:10.1063/1.5114928.
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Lee, Ilkeun, & Zaera, Francisco. Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO2 catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures. United States. https://doi.org/10.1063/1.5114928
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Lee, Ilkeun, and Zaera, Francisco. Thu . "Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO2 catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures". United States. https://doi.org/10.1063/1.5114928. https://www.osti.gov/servlets/purl/1593411.
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@article{osti_1593411,
title = {Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO2 catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures},
author = {Lee, Ilkeun and Zaera, Francisco},
abstractNote = {The ability of Au/TiO2 catalysts to promote the oxidation of carbon monoxide at cryogenic temperatures was probed by using diffuse-reflectance infrared absorption spectroscopy (DRIFTS). The aim of this work was to identify correlations between the catalytic activity and both the nature of the titania support and the size of the Au nanoparticles (NPs). Two key intermediates were identified: an initial CO adsorbed on defect sites within the titania support with a 2175 cm-1 C–O stretching frequency signature, and a second species with a DRIFTS peak at 2163 cm-1 associated with the intermediate at Au–TiO2 interfacial sites that incorporates atomic oxygen to produce CO2. CO adsorption at the low temperatures associated with this process (120 K) appears to require defective sites, possibly titanate-type surface species: an amorphous (and NaOH-treated) support showed higher activity than crystalline titania. Furthermore, the catalytic activity peaks at an Au NP average size of about 3 nm, which, in turn, correlates with the population of the second CO intermediate mentioned above. The mechanism that explains this cryogenic oxidation reaction is different than that extensively reported for the room-temperature processes, but both appear to display similar dependence on Au NP diameter.},
doi = {10.1063/1.5114928},
journal = {Journal of Chemical Physics},
number = 5,
volume = 151,
place = {United States},
year = {Thu Aug 01 00:00:00 EDT 2019},
month = {Thu Aug 01 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5114928
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Cited by: 8 works
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Figures / Tables:

Figure 1 Figure 1: TEM images of the 1.1 nm Au/TiO2-P25 catalyst and of the Au colloidal NPs with 3.2, 6.5, and 14.4 nm average diameters. Some of the Au NPs in the 1.1 nm case have been highlighted to better visualize them (white circles).
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    Works referencing / citing this record:

    Use of Au@Void@TiO 2 yolk-shell nanostructures to probe the influence of oxide crystallinity on catalytic activity for low-temperature oxidations
    journal, December 2019

    • Lee, Ilkeun; Zaera, Francisco
    • The Journal of Chemical Physics, Vol. 151, Issue 23
    • DOI: 10.1063/1.5132715
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