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

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.

doi:10.1021/acssuschemeng.7b02744

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), CO₃^2–(ads), and OH(ads) were identified under reaction conditions. CO₃^2–(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:

Palomino, Robert M. ^[1]; Gutiérrez, Ramón A. ^[2];

^[1]; Tenney, Samuel ^[1]; Grinter, David C. ^[1];

^[3]; Waluyo, Iradwikanari ^[1]; Ramírez, Pedro J. ^[2];

^[1];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. Central de Venezuela, Caracas (Venezuela)
Brookhaven National Lab. (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Publication Date:: 2017-09-26

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.  doi:10.1021/acssuschemeng.7b02744.

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                    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

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                    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.

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@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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https://doi.org/10.1021/acs.jpcc.6b11764

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Interfacial and Alloying Effects on Activation of Ethanol from First-Principles

Journal Article An, Wei ; Men, Yong ; Wang, Jinguo ; ... - Journal of Physical Chemistry. C

Here, we present a first-principles density-functional theory study of ethanol activation at oxide/Rh(111) interface and the alloying effect on mitigating carbon deposition, which are essential to direct ethanol fuel cell (DEFC) anode reaction and steam reforming of ethanol (SRE) reaction. Our calculated results show that charge can transfer from Rh(111) substrate to MO_x chain (e.g., MoO₃ and MnO₂), or from MO_x chain (e.g., MgO, SnO₂, ZrO₂, and TiO₂) to Rh(111) substrate. The OH-binding strength is increased exponentially with M^δ+ charge ranging from 1.4 to 2.2, which renders MnO₂/Rh(111) and MgO/Rh(111) interfaces weaker OH-binding, and thereby enhanced oxidizing functionality of OH*more »« less
Cited by 1
https://doi.org/10.1021/acs.jpcc.6b12720

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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)

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Citation Formats

Ionic Liquid-Assisted Sonochemical Preparation of CeO 2 Nanoparticles for CO Oxidation journal, December 2014

Tailoring metal–oxide interfaces of inverse catalysts of TiO 2 /nanoporous-Au under hydrogen oxidation journal, January 2015

Precisely Applying TiO 2 Overcoat on Supported Au Catalysts Using Atomic Layer Deposition for Understanding the Reaction Mechanism and Improved Activity in CO Oxidation journal, December 2015

Nanostructured Oxides in Chemistry: Characterization and Properties journal, September 2004

Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al 2 O 3 Catalysts Induced by Strong Metal-Support Interactions journal, February 2015

Promoting Strong Metal Support Interaction: Doping ZnO for Enhanced Activity of Cu/ZnO:M (M = Al, Ga, Mg) Catalysts journal, April 2015

In situ time-resolved characterization of novel Cu–MoO2 catalysts during the water–gas shift reaction journal, January 2007

Reversibility of strong metal-support interactions on Rh/TiO2 journal, July 1989

Support nanostructure boosts oxygen transfer to catalytically active platinum nanoparticles journal, March 2011

CO Oxidation on Gold-Supported Iron Oxides: New Insights into Strong Oxide–Metal Interactions journal, July 2015

Inverse CeO 2 /CuO Catalyst As an Alternative to Classical Direct Configurations for Preferential Oxidation of CO in Hydrogen-Rich Stream journal, January 2010

CO Oxidation on a CeO x /Pt(111) Inverse Model Catalyst Surface: Catalytic Promotion and Tuning of Kinetic Phase Diagrams journal, November 2008

CO oxidation on inverse Fe2O3/Au(111) model catalysts journal, October 2012

Adsorption and reaction of CO on a ceria–Rh(111) “inverse model catalyst” surface journal, June 2003

A Surface Science Investigation of Methanol Synthesis over a Zn-Deposited Polycrystalline Cu Surface journal, April 1996

Hydrogenation of CO 2 to Methanol on CeO x /Cu(111) and ZnO/Cu(111) Catalysts: Role of the Metal–Oxide Interface and Importance of Ce 3+ Sites journal, January 2016

Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2 journal, July 2014

Active sites for CO 2 hydrogenation to methanol on Cu/ZnO catalysts journal, March 2017

Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction journal, December 2007

Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy journal, April 2013

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

Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst journal, August 2011

Insights into Catalytic Oxidation at the Au/TiO 2 Dual Perimeter Sites journal, December 2013

Active gold-ceria and gold-ceria/titania catalysts for CO oxidation: From single-crystal model catalysts to powder catalysts journal, February 2015

Two-dimensional TiO x nanostructures on Au(111): a scanning tunneling microscopy and spectroscopy investigation journal, November 2015

Surface Structures of Ultrathin TiO x Films on Au(111) journal, April 2011

Formation of TiO 2 Nanoparticles by Reactive-Layer-Assisted Deposition and Characterization by XPS and STM journal, July 2005

Mechanism and Active Sites of the Oxidation of CO over Au/TiO2 journal, September 2011

Elucidation of Active Sites for the Reaction of Ethanol on TiO 2 /Au(111) journal, March 2017

Preparation of TiO 2 Nanocrystallites by Oxidation of Ti−Au(111) Surface Alloy journal, June 2009

Synthesis of TiO2 nanoparticles on the Au(111) surface journal, September 2005

Reaction of water with Ce–Au(111) and CeOx/Au(111) surfaces: Photoemission and STM studies journal, June 2007

Growth of Ceria Nano-Islands on a Stepped Au(788) Surface journal, August 2015

Competition between Polar and Nonpolar Growth of MgO Thin Films on Au(111) journal, October 2011

Compensating Edge Polarity: A Means To Alter the Growth Orientation of MgO Nanostructures on Au(111) journal, May 2012

New ambient pressure photoemission endstation at Advanced Light Source beamline 9.3.2 journal, May 2010

Adsorption and surface-enhanced Raman of dyes on silver and gold sols journal, August 1982

Effect of Ceria on Gold–Titania Catalysts for the Water–Gas Shift Reaction: Fundamental Studies for Au/CeO x /TiO 2 (110) and Au/CeO x /TiO 2 Powders journal, October 2012

Adsorption and Dissociation of O 2 on Gold Surfaces: Effect of Steps and Strain journal, September 2003

CO oxidation over Au/TiO2 catalyst: Pretreatment effects, catalyst deactivation, and carbonates production journal, November 2013

Stability and deactivation of unconditioned Au/TiO2 catalysts during CO oxidation in a near-stoichiometric and O2-rich reaction atmosphere journal, October 2007

High catalytic activity of Au/CeOx/TiO2(110) controlled by the nature of the mixed-metal oxide at the nanometer level journal, March 2009

Influence of TiO 2 Bulk Defects on CO Adsorption and CO Oxidation on Au/TiO 2 : Electronic Metal–Support Interactions (EMSIs) in Supported Au Catalysts journal, February 2017

Influence of Au Particle Size on Au/TiO 2 Catalysts for CO Oxidation journal, August 2014

Ultrathin metal films and particles on oxide surfaces: structural, electronic and chemisorptive properties journal, January 1997

Surface studies of supported model catalysts journal, January 1998

Electron Transfer at Oxide Surfaces. The MgO Paradigm: from Defects to Ultrathin Films journal, November 2012

Density functional study of water-gas shift reaction on M3O3x/Cu(111) journal, January 2012

Unraveling the Nature of the Oxide–Metal Interaction in Ceria-Based Noble Metal Inverse Catalysts journal, November 2014

XPS and FTIR Surface Characterization of TiO 2 Particles Used in Polymer Encapsulation journal, May 2001

Chemical reactions on rutile TiO2(110) journal, January 2008

CO Oxidation over Supported Gold Catalysts—“Inert” and “Active” Support Materials and Their Role for the Oxygen Supply during Reaction journal, January 2001

New insight of the Mars-van Krevelen mechanism of the CO oxidation by gold catalyst on the ZnO(101) surface journal, January 2017

In Situ Photoemission Observation of Catalytic CO Oxidation Reaction on Pd(110) under Near-Ambient Pressure Conditions: Evidence for the Langmuir–Hinshelwood Mechanism journal, September 2013

When Gold Is Not Noble: Catalysis by Nanoparticles journal, April 2003

Interaction of carbon monoxide and oxygen at the surface of inverse titania/Au model catalyst journal, July 2007

The critical role of water at the gold-titania interface in catalytic CO oxidation journal, September 2014

The Effect of Adsorbed Water in CO Oxidation on Au/TiO 2 (110) journal, December 2010

Morphology and reactivity of size-selected titanium oxide nanoclusters on Au(111) journal, February 2020

Growth and structural studies of In/Au(111) alloys and InO x /Au(111) inverse oxide/metal model catalysts journal, February 2020

CO Oxidation at 20 °C on Au Catalysts Supported on Mesoporous Silica: Effects of Support Structural Properties and Modifiers journal, June 2018

MOF-derived CeO 2 /Au@SiO 2 hollow nanotubes and their catalytic activity toward 4-nitrophenol reduction journal, January 2019

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

Ionic Liquid-Assisted Sonochemical Preparation of CeO ₂ Nanoparticles for CO Oxidation
journal, December 2014

Tailoring metal–oxide interfaces of inverse catalysts of TiO ₂ /nanoporous-Au under hydrogen oxidation
journal, January 2015

Precisely Applying TiO ₂ Overcoat on Supported Au Catalysts Using Atomic Layer Deposition for Understanding the Reaction Mechanism and Improved Activity in CO Oxidation
journal, December 2015

Nanostructured Oxides in Chemistry: Characterization and Properties
journal, September 2004

Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al ₂ O ₃ Catalysts Induced by Strong Metal-Support Interactions
journal, February 2015

Promoting Strong Metal Support Interaction: Doping ZnO for Enhanced Activity of Cu/ZnO:M (M = Al, Ga, Mg) Catalysts
journal, April 2015

In situ time-resolved characterization of novel Cu–MoO2 catalysts during the water–gas shift reaction
journal, January 2007

Reversibility of strong metal-support interactions on Rh/TiO2
journal, July 1989

Support nanostructure boosts oxygen transfer to catalytically active platinum nanoparticles
journal, March 2011

CO Oxidation on Gold-Supported Iron Oxides: New Insights into Strong Oxide–Metal Interactions
journal, July 2015

Inverse CeO ₂ /CuO Catalyst As an Alternative to Classical Direct Configurations for Preferential Oxidation of CO in Hydrogen-Rich Stream
journal, January 2010

CO Oxidation on a CeO _x /Pt(111) Inverse Model Catalyst Surface: Catalytic Promotion and Tuning of Kinetic Phase Diagrams
journal, November 2008

CO oxidation on inverse Fe2O3/Au(111) model catalysts
journal, October 2012

Adsorption and reaction of CO on a ceria–Rh(111) “inverse model catalyst” surface
journal, June 2003

A Surface Science Investigation of Methanol Synthesis over a Zn-Deposited Polycrystalline Cu Surface
journal, April 1996

Hydrogenation of CO ₂ to Methanol on CeO _x /Cu(111) and ZnO/Cu(111) Catalysts: Role of the Metal–Oxide Interface and Importance of Ce ³⁺ Sites
journal, January 2016

Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2
journal, July 2014

Active sites for CO ₂ hydrogenation to methanol on Cu/ZnO catalysts
journal, March 2017

Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction
journal, December 2007

Importance of the Metal-Oxide Interface in Catalysis: In Situ Studies of the Water-Gas Shift Reaction by Ambient-Pressure X-ray Photoelectron Spectroscopy
journal, April 2013

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

Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst
journal, August 2011

Insights into Catalytic Oxidation at the Au/TiO ₂ Dual Perimeter Sites
journal, December 2013

Active gold-ceria and gold-ceria/titania catalysts for CO oxidation: From single-crystal model catalysts to powder catalysts
journal, February 2015

Two-dimensional TiO _x nanostructures on Au(111): a scanning tunneling microscopy and spectroscopy investigation
journal, November 2015

Surface Structures of Ultrathin TiO _x Films on Au(111)
journal, April 2011

Formation of TiO ₂ Nanoparticles by Reactive-Layer-Assisted Deposition and Characterization by XPS and STM
journal, July 2005

Mechanism and Active Sites of the Oxidation of CO over Au/TiO2
journal, September 2011

Elucidation of Active Sites for the Reaction of Ethanol on TiO ₂ /Au(111)
journal, March 2017

Preparation of TiO ₂ Nanocrystallites by Oxidation of Ti−Au(111) Surface Alloy
journal, June 2009

Synthesis of TiO2 nanoparticles on the Au(111) surface
journal, September 2005

Reaction of water with Ce–Au(111) and CeOx/Au(111) surfaces: Photoemission and STM studies
journal, June 2007

Growth of Ceria Nano-Islands on a Stepped Au(788) Surface
journal, August 2015

Competition between Polar and Nonpolar Growth of MgO Thin Films on Au(111)
journal, October 2011

Compensating Edge Polarity: A Means To Alter the Growth Orientation of MgO Nanostructures on Au(111)
journal, May 2012

New ambient pressure photoemission endstation at Advanced Light Source beamline 9.3.2
journal, May 2010

Adsorption and surface-enhanced Raman of dyes on silver and gold sols
journal, August 1982

Effect of Ceria on Gold–Titania Catalysts for the Water–Gas Shift Reaction: Fundamental Studies for Au/CeO _x /TiO ₂ (110) and Au/CeO _x /TiO ₂ Powders
journal, October 2012

Adsorption and Dissociation of O ₂ on Gold Surfaces: Effect of Steps and Strain
journal, September 2003

CO oxidation over Au/TiO2 catalyst: Pretreatment effects, catalyst deactivation, and carbonates production
journal, November 2013

Stability and deactivation of unconditioned Au/TiO2 catalysts during CO oxidation in a near-stoichiometric and O2-rich reaction atmosphere
journal, October 2007

High catalytic activity of Au/CeOx/TiO2(110) controlled by the nature of the mixed-metal oxide at the nanometer level
journal, March 2009

Influence of TiO ₂ Bulk Defects on CO Adsorption and CO Oxidation on Au/TiO ₂ : Electronic Metal–Support Interactions (EMSIs) in Supported Au Catalysts
journal, February 2017

Influence of Au Particle Size on Au/TiO ₂ Catalysts for CO Oxidation
journal, August 2014

Ultrathin metal films and particles on oxide surfaces: structural, electronic and chemisorptive properties
journal, January 1997

Surface studies of supported model catalysts
journal, January 1998

Electron Transfer at Oxide Surfaces. The MgO Paradigm: from Defects to Ultrathin Films
journal, November 2012

Density functional study of water-gas shift reaction on M3O3x/Cu(111)
journal, January 2012

Unraveling the Nature of the Oxide–Metal Interaction in Ceria-Based Noble Metal Inverse Catalysts
journal, November 2014

XPS and FTIR Surface Characterization of TiO ₂ Particles Used in Polymer Encapsulation
journal, May 2001

Chemical reactions on rutile TiO2(110)
journal, January 2008

CO Oxidation over Supported Gold Catalysts—“Inert” and “Active” Support Materials and Their Role for the Oxygen Supply during Reaction
journal, January 2001

New insight of the Mars-van Krevelen mechanism of the CO oxidation by gold catalyst on the ZnO(101) surface
journal, January 2017

In Situ Photoemission Observation of Catalytic CO Oxidation Reaction on Pd(110) under Near-Ambient Pressure Conditions: Evidence for the Langmuir–Hinshelwood Mechanism
journal, September 2013

When Gold Is Not Noble: Catalysis by Nanoparticles
journal, April 2003

Interaction of carbon monoxide and oxygen at the surface of inverse titania/Au model catalyst
journal, July 2007

The critical role of water at the gold-titania interface in catalytic CO oxidation
journal, September 2014

The Effect of Adsorbed Water in CO Oxidation on Au/TiO ₂ (110)
journal, December 2010

Morphology and reactivity of size-selected titanium oxide nanoclusters on Au(111)
journal, February 2020

Growth and structural studies of In/Au(111) alloys and InO _x /Au(111) inverse oxide/metal model catalysts
journal, February 2020

CO Oxidation at 20 °C on Au Catalysts Supported on Mesoporous Silica: Effects of Support Structural Properties and Modifiers
journal, June 2018

MOF-derived CeO ₂ /Au@SiO ₂ hollow nanotubes and their catalytic activity toward 4-nitrophenol reduction
journal, January 2019