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Title: Investigation of the Origin of Catalytic Activity in Oxide-Supported Nanoparticle Gold

Abstract

Since Haruta’s discovery in 1987 of the surprising catalytic activity of supported Au nanoparticles, we have seen a very large number of experimental and theoretical efforts to explain this activity and to fully understand the nature of the behavior of the responsible active sites. In 2011, we discovered that a dual catalytic site at the perimeter of ~3nm diameter Au particles supported on TiO 2 is responsible for oxidative catalytic activity. O 2 molecules bind with Au atoms and Ti4+ ions in the TiO 2 support and the weakened O-O bond dissociates at low temperatures, proceeding to produce O atoms which act as oxidizing agents for the test molecule, CO. The papers supported by DOE have built on this finding and have been concerned with two aspects of the behavior of Au/TiO 2 catalysts: (1). Mechanistic behavior of dual catalytic sites in the oxidation of organic molecules such as ethylene and acetic acid; (2). Studies of the electronic properties of the TiO 2 (110) single crystal in relation to its participation in charge transfer at the occupied dual catalytic site. A total of 20 papers have been produced through DOE support of this work. The papers combine IR spectroscopic investigationsmore » of Au/TiO 2 catalysts with surface science on the TiO 2(110) and TiO 2 nanoparticle surfaces with modern density functional modeling. The primary goals of the work were to investigate the behavior of the dual Au/Ti 4+ site for the partial oxidation of alcohols to acids, the hydrogenation of aldehydes and ketones to alcohols, and the condensation of oxygenate intermediates- all processes related to the utilization of biomass in the production of useful chemical energy sources.« less

Authors:
 [1]
  1. Univ. of Virginia, Charlottesville, VA (United States)
Publication Date:
Research Org.:
Univ. of Virginia, Charlottesville, VA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1358579
Report Number(s):
DOE-UVA-0002365
DOE Contract Number:  
SC0002365
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 09 BIOMASS FUELS; 74 ATOMIC AND MOLECULAR PHYSICS; 77 NANOSCIENCE AND NANOTECHNOLOGY; catalysis; heterogenous catalysis; TiO2; gold catalysis; nanoparticles; reaction mechanism; active sites

Citation Formats

Harrison, Ian. Investigation of the Origin of Catalytic Activity in Oxide-Supported Nanoparticle Gold. United States: N. p., 2017. Web. doi:10.2172/1358579.
Harrison, Ian. Investigation of the Origin of Catalytic Activity in Oxide-Supported Nanoparticle Gold. United States. doi:10.2172/1358579.
Harrison, Ian. Fri . "Investigation of the Origin of Catalytic Activity in Oxide-Supported Nanoparticle Gold". United States. doi:10.2172/1358579. https://www.osti.gov/servlets/purl/1358579.
@article{osti_1358579,
title = {Investigation of the Origin of Catalytic Activity in Oxide-Supported Nanoparticle Gold},
author = {Harrison, Ian},
abstractNote = {Since Haruta’s discovery in 1987 of the surprising catalytic activity of supported Au nanoparticles, we have seen a very large number of experimental and theoretical efforts to explain this activity and to fully understand the nature of the behavior of the responsible active sites. In 2011, we discovered that a dual catalytic site at the perimeter of ~3nm diameter Au particles supported on TiO2 is responsible for oxidative catalytic activity. O2 molecules bind with Au atoms and Ti4+ ions in the TiO2 support and the weakened O-O bond dissociates at low temperatures, proceeding to produce O atoms which act as oxidizing agents for the test molecule, CO. The papers supported by DOE have built on this finding and have been concerned with two aspects of the behavior of Au/TiO2 catalysts: (1). Mechanistic behavior of dual catalytic sites in the oxidation of organic molecules such as ethylene and acetic acid; (2). Studies of the electronic properties of the TiO2 (110) single crystal in relation to its participation in charge transfer at the occupied dual catalytic site. A total of 20 papers have been produced through DOE support of this work. The papers combine IR spectroscopic investigations of Au/TiO2 catalysts with surface science on the TiO2(110) and TiO2 nanoparticle surfaces with modern density functional modeling. The primary goals of the work were to investigate the behavior of the dual Au/Ti4+ site for the partial oxidation of alcohols to acids, the hydrogenation of aldehydes and ketones to alcohols, and the condensation of oxygenate intermediates- all processes related to the utilization of biomass in the production of useful chemical energy sources.},
doi = {10.2172/1358579},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri May 26 00:00:00 EDT 2017},
month = {Fri May 26 00:00:00 EDT 2017}
}

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