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Title: Inverse Catalysts for CO Oxidation: Enhanced Oxide–Metal Interactions in MgO/Au(111), CeO2/Au(111), and TiO2/Au(111)

Abstract

Au(111) does not bind CO and O2 well. The deposition of small nanoparticles of MgO, CeO2, and TiO2 on Au(111) produces excellent catalysts for CO oxidation at room temperature. In an inverse oxide/metal configuration there is a strong enhancement of the oxide–metal interactions, and the inverse catalysts are more active than conventional Au/MgO(001), Au/CeO2(111), and Au/TiO2(110) catalysts. An identical trend was seen after comparing the CO oxidation activity of TiO2/Au and Au/TiO2 powder catalysts. In the model systems, the activity increased following the sequence: MgO/Au(111) < CeO2/Au(111) < TiO2/Au(111). Ambient pressure X-ray photoelectron spectroscopy (AP-XPS) was used to elucidate the role of the titania–gold interface in inverse TiO2/Au(111) model catalysts during CO oxidation. Stable surface intermediates such as CO(ads), CO32–(ads), and OH(ads) were identified under reaction conditions. CO32–(ads) and OH(ads) behaved as spectators. The concentration of CO(ad) initially increased and then decreased with increasing TiO2 coverage, demonstrating a clear role of the Ti–Au interface and the size of the TiO2 nanostructures in the catalytic process. Overall, our results show an enhancement in the strength of the oxide–metal interactions when working with inverse oxide/metal configurations, a phenomenon that can be utilized for the design of efficient catalysts useful for green andmore » sustainable chemistry.« less

Authors:
 [1];  [2]; ORCiD logo [1];  [1];  [1]; ORCiD logo [3];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Univ. Central de Venezuela, Caracas (Venezuela)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1425036
Report Number(s):
BNL-200017-2018-JAAM
Journal ID: ISSN 2168-0485
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 5; Journal Issue: 11; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Palomino, Robert M., Gutiérrez, Ramón A., Liu, Zongyuan, Tenney, Samuel, Grinter, David C., Crumlin, Ethan, Waluyo, Iradwikanari, Ramírez, Pedro J., Rodriguez, José A., and Senanayake, Sanjaya D. Inverse Catalysts for CO Oxidation: Enhanced Oxide–Metal Interactions in MgO/Au(111), CeO2/Au(111), and TiO2/Au(111). United States: N. p., 2017. Web. https://doi.org/10.1021/acssuschemeng.7b02744.
Palomino, Robert M., Gutiérrez, Ramón A., Liu, Zongyuan, Tenney, Samuel, Grinter, David C., Crumlin, Ethan, Waluyo, Iradwikanari, Ramírez, Pedro J., Rodriguez, José A., & Senanayake, Sanjaya D. Inverse Catalysts for CO Oxidation: Enhanced Oxide–Metal Interactions in MgO/Au(111), CeO2/Au(111), and TiO2/Au(111). United States. https://doi.org/10.1021/acssuschemeng.7b02744
Palomino, Robert M., Gutiérrez, Ramón A., Liu, Zongyuan, Tenney, Samuel, Grinter, David C., Crumlin, Ethan, Waluyo, Iradwikanari, Ramírez, Pedro J., Rodriguez, José A., and Senanayake, Sanjaya D. Tue . "Inverse Catalysts for CO Oxidation: Enhanced Oxide–Metal Interactions in MgO/Au(111), CeO2/Au(111), and TiO2/Au(111)". United States. https://doi.org/10.1021/acssuschemeng.7b02744. https://www.osti.gov/servlets/purl/1425036.
@article{osti_1425036,
title = {Inverse Catalysts for CO Oxidation: Enhanced Oxide–Metal Interactions in MgO/Au(111), CeO2/Au(111), and TiO2/Au(111)},
author = {Palomino, Robert M. and Gutiérrez, Ramón A. and Liu, Zongyuan and Tenney, Samuel and Grinter, David C. and Crumlin, Ethan and Waluyo, Iradwikanari and Ramírez, Pedro J. and Rodriguez, José A. and Senanayake, Sanjaya D.},
abstractNote = {Au(111) does not bind CO and O2 well. The deposition of small nanoparticles of MgO, CeO2, and TiO2 on Au(111) produces excellent catalysts for CO oxidation at room temperature. In an inverse oxide/metal configuration there is a strong enhancement of the oxide–metal interactions, and the inverse catalysts are more active than conventional Au/MgO(001), Au/CeO2(111), and Au/TiO2(110) catalysts. An identical trend was seen after comparing the CO oxidation activity of TiO2/Au and Au/TiO2 powder catalysts. In the model systems, the activity increased following the sequence: MgO/Au(111) < CeO2/Au(111) < TiO2/Au(111). Ambient pressure X-ray photoelectron spectroscopy (AP-XPS) was used to elucidate the role of the titania–gold interface in inverse TiO2/Au(111) model catalysts during CO oxidation. Stable surface intermediates such as CO(ads), CO32–(ads), and OH(ads) were identified under reaction conditions. CO32–(ads) and OH(ads) behaved as spectators. The concentration of CO(ad) initially increased and then decreased with increasing TiO2 coverage, demonstrating a clear role of the Ti–Au interface and the size of the TiO2 nanostructures in the catalytic process. Overall, our results show an enhancement in the strength of the oxide–metal interactions when working with inverse oxide/metal configurations, a phenomenon that can be utilized for the design of efficient catalysts useful for green and sustainable chemistry.},
doi = {10.1021/acssuschemeng.7b02744},
journal = {ACS Sustainable Chemistry & Engineering},
number = 11,
volume = 5,
place = {United States},
year = {2017},
month = {9}
}

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