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

He, Qian; Freakley, Simon J.; Edwards, Jennifer K.; Carley, Albert F.; Borisevich, Albina Y.; Mineo, Yuki; Haruta, Masatake; Hutchings, Graham J.; Kiely, Christopher J.

doi:10.1038/ncomms12905

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:

He, Qian ^[1]; Freakley, Simon J. ^[2]; Edwards, Jennifer K. ^[2]; Carley, Albert F. ^[2]; Borisevich, Albina Y. ^[3]; Mineo, Yuki ^[4]; Haruta, Masatake ^[4]; Hutchings, Graham J. ^[2]; Kiely, Christopher J. ^[5]

Lehigh Univ., Bethlehem, PA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Cardiff Univ., Cardiff (United Kingdom)
Cardiff Univ., Cardiff (United Kingdom)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Tokyo Metropolitan Univ., Tokyo (Japan)
Lehigh Univ., Bethlehem, PA (United States)

Publication Date:: Tue Sep 27 00:00:00 EDT 2016

Research Org.:: Oak Ridge National Lab. (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.

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                    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.  https://doi.org/10.1038/ncomms12905

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                    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. 2016.  
        "Population and hierarchy of active species in gold iron oxide catalysts for carbon monoxide oxidation".  United States.  https://doi.org/10.1038/ncomms12905.  https://www.osti.gov/servlets/purl/1329164.

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@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},

  url          = {https://www.osti.gov/biblio/1329164},
  journal      = {Nature Communications},

  issn         = {2041-1723},

  number       = ,

  volume       = 7,

  place        = {United States},

  year         = {Tue Sep 27 00:00:00 EDT 2016},

  month        = {Tue Sep 27 00:00:00 EDT 2016}

}

Copy to clipboard

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Similar Records

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

Abstract

Citation Formats

High-activity Au/CuO–ZnO catalysts for the oxidation of carbon monoxide at ambient temperature journal, January 1997

On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation journal, April 2004

Behavior of Au Species in Au/FeOx Catalysts as a Result of In-Situ Thermal Treatments, Characterized via Aberration-Corrected STEM Imaging journal, July 2009

Size- and Structure-specificity in Catalysis by Gold Clusters journal, April 2014

Hydrogenation of m-dinitrobenzene over Au catalysts on magnetic supports journal, March 2014

Gold Catalysis journal, December 2006

Gold-Iron Oxide Catalyst for CO Oxidation: Effect of Support Structure journal, March 2016

New Strategies for Controlling the Size, Morphology and Composition of Bimetallic and Trimetallic Catalyst Particles journal, August 2013

Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: structure–activity relationship journal, January 2015

Factors in gold nanocatalysis: oxidation of CO in the non-scalable size regime journal, June 2007

Gold catalysts prepared by coprecipitation for low-temperature oxidation of hydrogen and of carbon monoxide journal, February 1989

Low temperature reductive pretreatment of Au/Fe2O3 catalysts, TPR/TPO studies and behaviour in the water–gas shift reaction journal, February 2004

Size- and support-dependency in the catalysis of gold journal, April 1997

Low-Temperature Oxidation of CO over Gold Supported on TiO2, α-Fe2O3, and Co3O4 journal, November 1993

Highly Active Iron Oxide Supported Gold Catalysts for CO Oxidation: How Small Must the Gold Nanoparticles Be? journal, July 2010

Kinetics of CO oxidation catalyzed by highly dispersed CeO2-supported gold journal, December 2008

Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C journal, February 1987

Au/iron oxide catalysts: temperature programmed reduction and X-ray diffraction characterization journal, April 1999

Evolution of gold structure during thermal treatment of Au/FeOx catalysts revealed by aberration-corrected electron microscopy journal, April 2009

Size effect on the melting temperature of gold particles journal, June 1976

Direct formation of hydrogen peroxide from H2/O2 using a gold catalyst journal, August 2002

Catalytically active gold on ordered titania supports journal, January 2008

Spiers Memorial Lecture : Role of perimeter interfaces in catalysis by gold nanoparticles journal, January 2011

Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation journal, September 2008

Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI) journal, July 2015

Onset of Catalytic Activity of Gold Clusters on Titania with the Appearance of Nonmetallic Properties journal, September 1998

Gold-catalysed oxidation of carbon monoxide journal, June 2000

A dense non-crystallographic packing of equal spheres journal, September 1962

Gold Catalysis journal, March 2007

Highly Active Iron Oxide Supported Gold Catalysts for CO Oxidation: How Small Must the Gold Nanoparticles Be? journal, July 2010

Factors in Gold Nanocatalysis: Oxidation of CO in the Non-Scalable Size Regime journal, November 2007

Sub nanometer clusters in catalysis journal, November 2018

Nanostructured Metal Catalysts for Selective Hydrogenation and Oxidation of Cellulosic Biomass to Chemicals journal, November 2018

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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

Acetylene hydrochlorination using Au/carbon: a journey towards single site catalysis journal, January 2017

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

High-activity Au/CuO–ZnO catalysts for the oxidation of carbon monoxide at ambient temperature
journal, January 1997

On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation
journal, April 2004

Behavior of Au Species in Au/FeOx Catalysts as a Result of In-Situ Thermal Treatments, Characterized via Aberration-Corrected STEM Imaging
journal, July 2009

Size- and Structure-specificity in Catalysis by Gold Clusters
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Factors in gold nanocatalysis: oxidation of CO in the non-scalable size regime
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Gold catalysts prepared by coprecipitation for low-temperature oxidation of hydrogen and of carbon monoxide
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Low temperature reductive pretreatment of Au/Fe2O3 catalysts, TPR/TPO studies and behaviour in the water–gas shift reaction
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Size- and support-dependency in the catalysis of gold
journal, April 1997

Low-Temperature Oxidation of CO over Gold Supported on TiO2, α-Fe2O3, and Co3O4
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Highly Active Iron Oxide Supported Gold Catalysts for CO Oxidation: How Small Must the Gold Nanoparticles Be?
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Kinetics of CO oxidation catalyzed by highly dispersed CeO2-supported gold
journal, December 2008

Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C
journal, February 1987

Au/iron oxide catalysts: temperature programmed reduction and X-ray diffraction characterization
journal, April 1999

Evolution of gold structure during thermal treatment of Au/FeOx catalysts revealed by aberration-corrected electron microscopy
journal, April 2009

Size effect on the melting temperature of gold particles
journal, June 1976

Direct formation of hydrogen peroxide from H2/O2 using a gold catalyst
journal, August 2002

Catalytically active gold on ordered titania supports
journal, January 2008

Spiers Memorial Lecture : Role of perimeter interfaces in catalysis by gold nanoparticles
journal, January 2011

Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation
journal, September 2008

Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI)
journal, July 2015

Onset of Catalytic Activity of Gold Clusters on Titania with the Appearance of Nonmetallic Properties
journal, September 1998

Gold-catalysed oxidation of carbon monoxide
journal, June 2000

A dense non-crystallographic packing of equal spheres
journal, September 1962

Gold Catalysis
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Highly Active Iron Oxide Supported Gold Catalysts for CO Oxidation: How Small Must the Gold Nanoparticles Be?
journal, July 2010

Factors in Gold Nanocatalysis: Oxidation of CO in the Non-Scalable Size Regime
journal, November 2007

Sub nanometer clusters in catalysis
journal, November 2018

Nanostructured Metal Catalysts for Selective Hydrogenation and Oxidation of Cellulosic Biomass to Chemicals
journal, November 2018

Strategies for Stabilizing Atomically Dispersed Metal Catalysts
journal, December 2017

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

Acetylene hydrochlorination using Au/carbon: a journey towards single site catalysis
journal, January 2017

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