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

Abstract

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/FeO x 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/FeO x catalyst.

Authors:
 [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)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE
OSTI Identifier:
1329164
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst synthesis; heterogeneous catalysis

Citation Formats

He, Qian, Freakley, Simon J., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Mineo, Yuki, Haruta, Masatake, Hutchings, Graham J., and Kiely, Christopher J. Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation. United States: N. p., 2016. Web. doi:10.1038/ncomms12905.
He, Qian, Freakley, Simon J., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Mineo, Yuki, Haruta, Masatake, Hutchings, Graham J., & Kiely, Christopher J. Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation. United States. doi:10.1038/ncomms12905.
He, Qian, Freakley, Simon J., Edwards, Jennifer K., Carley, Albert F., Borisevich, Albina Y., Mineo, Yuki, Haruta, Masatake, Hutchings, Graham J., and Kiely, Christopher J. Tue . "Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation". United States. doi:10.1038/ncomms12905. https://www.osti.gov/servlets/purl/1329164.
@article{osti_1329164,
title = {Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation},
author = {He, Qian and Freakley, Simon J. and Edwards, Jennifer K. and Carley, Albert F. and Borisevich, Albina Y. and Mineo, Yuki and Haruta, Masatake and Hutchings, Graham J. and Kiely, Christopher J.},
abstractNote = {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.},
doi = {10.1038/ncomms12905},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue Sep 27 00:00:00 EDT 2016},
month = {Tue Sep 27 00:00:00 EDT 2016}
}

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Cited by: 6 works
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