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Title: Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms12905· OSTI ID:1329164
 [1];  [2];  [2];  [2];  [3];  [4];  [4];  [2];  [5]
  1. Lehigh Univ., Bethlehem, PA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Cardiff Univ., Cardiff (United Kingdom)
  2. Cardiff Univ., Cardiff (United Kingdom)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Tokyo Metropolitan Univ., Tokyo (Japan)
  5. Lehigh Univ., Bethlehem, PA (United States)

The identity of active species in supported gold catalysts for low temperature carbon monoxide oxidation remains an unsettled debate. With large amounts of experimental evidence supporting theories of either gold nanoparticles or sub-nm gold species being active, it was recently proposed that a size-dependent activity hierarchy should exist. Here we study the diverging catalytic behaviors after heat treatment of Au/FeOx materials prepared via co-precipitation and deposition precipitation methods. After ruling out any support effects, the gold particle size distributions in different catalysts are quantitatively studied using aberration corrected scanning transmission electron microscopy (STEM). A counting protocol is developed to reveal the true particle size distribution from HAADF-STEM images, which reliably includes all the gold species present. As a result, correlation of the populations of the various gold species present with catalysis results demonstrate that a size-dependent activity hierarchy must exist in the Au/FeOx catalyst.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1329164
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 55 works
Citation information provided by
Web of Science

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Activation and Deactivation of Gold/Ceria-Zirconia in the Low-Temperature Water-Gas Shift Reaction journal November 2017
Abnormal thermal stability of sub-10 nm Au nanoparticles and their high catalytic activity journal January 2019
Thermodynamics of faceted palladium(–gold) nanoparticles supported on rutile titania nanorods studied using transmission electron microscopy journal January 2018
Ultra-stable metal nano-catalyst synthesis strategy: a perspective journal December 2019
Aerobic Toluene Oxidation Catalyzed by Subnano Metal Particles journal December 2018
Activation and Deactivation of Gold/Ceria–Zirconia in the Low‐Temperature Water–Gas Shift Reaction journal November 2017
Aerobic Toluene Oxidation Catalyzed by Subnano Metal Particles journal December 2018