Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Matsubu, John C.; Zhang, Shuyi; DeRita, Leo; Marinkovic, Nebojsa S.; Chen, Jingguang G.; Graham, George W.; Pan, Xiaoqing; Christopher, Phillip

doi:10.1038/NCHEM.2607

Title: Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Abstract

The optimization of supported metal catalysts predominantly focuses on engineering the metal site, for which physical insights based on extensive theoretical and experimental contributions have enabled the rational design of active sites. Although it is well known that supports can influence the catalytic properties of metals, insights into how metal–support interactions can be exploited to optimize metal active-site properties are lacking. Here in this paper, we utilize in situ spectroscopy and microscopy to identify and characterize a support effect in oxide-supported heterogeneous Rh catalysts. This effect is characterized by strongly bound adsorbates (HCO_x) on reducible oxide supports (TiO₂ and Nb₂O₅) that induce oxygen-vacancy formation in the support and cause HCO_x-functionalized encapsulation of Rh nanoparticles by the support. The encapsulation layer is permeable to reactants, stable under the reaction conditions and strongly influences the catalytic properties of Rh, which enables rational and dynamic tuning of CO₂-reduction selectivity.

Authors:

Matsubu, John C. ^[1]; Zhang, Shuyi ^[2]; DeRita, Leo ^[1]; Marinkovic, Nebojsa S. ^[3]; Chen, Jingguang G. ^[4]; Graham, George W. ^[2]; Pan, Xiaoqing ^[5]; Christopher, Phillip ^[6]

University of California, Riverside, CA (United States). Department of Chemical and Environmental Engineering
University of California, Irvine, CA (United States). Department of Chemical Engineering and Materials Science; Univ. of Michigan, Ann Arbor, MI (United States). Department of Materials Science and Engineering
Columbia Univ., New York, NY (United States). Department of Chemical Engineering,
Columbia Univ., New York, NY (United States). Department of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
University of California, Irvine, CA (United States). Department of Chemical Engineering and Materials Science and Department of Physics and Astronomy
University of California, Riverside, CA (United States). Department of Chemical and Environmental Engineering, Program in Materials Science, and UCR Center for Catalysis

Publication Date:: Mon Sep 19 00:00:00 EDT 2016

Research Org.:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1358016

Report Number(s):: BNL-113828-2017-JA
Journal ID: ISSN 1755-4330; R&D Project: CO035; KC0302010

Grant/Contract Number:: SC0012704; SC0012335; CHE-1301019; CBET-1159240; DMR-0723032

Resource Type:: Accepted Manuscript

Journal Name:: Nature Chemistry

Additional Journal Information:: Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 1755-4330

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalytic mechanisms; Heterogeneous catalysis

Citation Formats


                    Matsubu, John C., Zhang, Shuyi, DeRita, Leo, Marinkovic, Nebojsa S., Chen, Jingguang G., Graham, George W., Pan, Xiaoqing, and Christopher, Phillip. Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts.  United States: N. p., 2016. 
Web.  doi:10.1038/NCHEM.2607.

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                    Matsubu, John C., Zhang, Shuyi, DeRita, Leo, Marinkovic, Nebojsa S., Chen, Jingguang G., Graham, George W., Pan, Xiaoqing, & Christopher, Phillip. Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts.  United States.  https://doi.org/10.1038/NCHEM.2607

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                    Matsubu, John C., Zhang, Shuyi, DeRita, Leo, Marinkovic, Nebojsa S., Chen, Jingguang G., Graham, George W., Pan, Xiaoqing, and Christopher, Phillip. Mon .  
"Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts".  United States.  https://doi.org/10.1038/NCHEM.2607.  https://www.osti.gov/servlets/purl/1358016.

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@article{osti_1358016,

  title        = {Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts},

  author       = {Matsubu, John C. and Zhang, Shuyi and DeRita, Leo and Marinkovic, Nebojsa S. and Chen, Jingguang G. and Graham, George W. and Pan, Xiaoqing and Christopher, Phillip},

  abstractNote = {The optimization of supported metal catalysts predominantly focuses on engineering the metal site, for which physical insights based on extensive theoretical and experimental contributions have enabled the rational design of active sites. Although it is well known that supports can influence the catalytic properties of metals, insights into how metal–support interactions can be exploited to optimize metal active-site properties are lacking. Here in this paper, we utilize in situ spectroscopy and microscopy to identify and characterize a support effect in oxide-supported heterogeneous Rh catalysts. This effect is characterized by strongly bound adsorbates (HCOx) on reducible oxide supports (TiO2 and Nb2O5) that induce oxygen-vacancy formation in the support and cause HCOx-functionalized encapsulation of Rh nanoparticles by the support. The encapsulation layer is permeable to reactants, stable under the reaction conditions and strongly influences the catalytic properties of Rh, which enables rational and dynamic tuning of CO2-reduction selectivity.},

  doi          = {10.1038/NCHEM.2607},

  journal      = {Nature Chemistry},

  number       = 2,

  volume       = 9,

  place        = {United States},

  year         = {Mon Sep 19 00:00:00 EDT 2016},

  month        = {Mon Sep 19 00:00:00 EDT 2016}

}

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High‐Performance Ultrathin Co ₃ O ₄ Nanosheet Supported PdO/CeO ₂ Catalysts for Methane Combustion
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Li, Wang; Liu, Dapeng; Feng, Xilan
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Jiang, Nan; Zhou, Xiao; Jiang, Yi-Fan
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Oxidative strong metal–support interactions (OMSI) of supported platinum-group metal catalysts
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Title: Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts

Abstract

Citation Formats

Isolated Metal Active Site Concentration and Stability Control Catalytic CO 2 Reduction Selectivity journal, February 2015

Trends in the catalytic reduction of CO2 by hydrogen over supported monometallic and bimetallic catalysts journal, May 2013

Counting electrons on supported nanoparticles journal, December 2015

Zeolite-Supported Rhodium Complexes and Clusters: Switching Catalytic Selectivity by Controlling Structures of Essentially Molecular Species journal, April 2011

Dynamic structural evolution of supported palladium–ceria core–shell catalysts revealed by in situ electron microscopy journal, July 2015

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Catalytic reduction of CO 2 by H 2 for synthesis of CO, methanol and hydrocarbons: challenges and opportunities journal, January 2016

Comparison of Metal-Support Interactions in Pt/TiO2 and Pt/CeO2 journal, August 1995

Real-space observation of strong metal-support interaction: state-of-the-art and what's the next: REAL-SPACE OBSERVATION OF STRONG METAL-SUPPORT INTERACTION journal, December 2015

Effect of NO on the CO-induced disruption of rhodium crystallites journal, July 1988

EXAFS evidence for direct metal-metal bonding in reduced rhodium/titania catalysts journal, April 1986

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

Metal-Support Interactions in Rh/CeO2, Rh/TiO2, and Rh/Nb2O5 Catalysts as Inferred from CO2 Methanation Activity journal, September 1995

Promotion of CO and CO2 Hydrogenation over Rh by Metal Oxides: The Influence of Oxide Lewis Acidity and Reducibility journal, September 1994

An infrared study of the hydrogenation of carbon dioxide on supported rhodium catalysts journal, April 1985

High-performance Ag–Co alloy catalysts for electrochemical oxygen reduction journal, August 2014

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

In-situ FT-IR study on CO2 hydrogenation over Cu catalysts supported on SiO2, Al2O3, and TiO2 journal, December 1997

Dynamical Observation and Detailed Description of Catalysts under Strong Metal–Support Interaction journal, June 2016

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide journal, January 1978

Multiple-scattering calculations of x-ray-absorption spectra journal, July 1995

IFEFFIT : interactive XAFS analysis and FEFF fitting journal, March 2001

Influence of Dipole–Dipole Interactions on Coverage-Dependent Adsorption: CO and NO on Pt(111) journal, May 2012

Probing Terrace and Step Sites on Pt Nanoparticles Using CO and Ethylene journal, April 2010

Magnetosomes could be protective shields against metal stress in magnetotactic bacteria journal, July 2020

Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol journal, March 2014

Finding optimal surface sites on heterogeneous catalysts by counting nearest neighbors journal, October 2015

Engineering Selectivity in Heterogeneous Catalysis: Ag Nanowires as Selective Ethylene Epoxidation Catalysts journal, August 2008

Charge Transfer in Metal Catalysts Supported on Doped TiO2: A Theoretical Approach Based on Metal–Semiconductor Contact Theory journal, July 1996

Some contributions of electron microscopy to the characterisation of the strong metal–support interaction effect journal, January 2003

Revealing particle growth mechanisms by combining high-surface-area catalysts made with monodisperse particles and electron microscopy conducted at atmospheric pressure journal, May 2016

Selective methanation of CO over supported noble metal catalysts: Effects of the nature of the metallic phase on catalytic performance journal, July 2008

Direct observation of the surfaces of small metal crystallites: rhodium supported on titania journal, July 1988

The surface science of titanium dioxide journal, January 2003

A versatile sample-environment cell for non-ambient X-ray scattering experiments journal, July 2008

Mechanism of CO2 reduction by H2 on Ru(0 0 0 1) and general selectivity descriptors for late-transition metal catalysts journal, November 2016

First-Principles Theoretical Study and Scanning Tunneling Microscopic Observation of Dehydration Process of Formic Acid on a TiO 2 (110) Surface † journal, September 2004

Metal-support effects on the intramolecular selectivity of crotonaldehyde hydrogenation over platinum journal, January 1989

Electronic perturbations journal, July 2012

A New Type of Strong Metal–Support Interaction and the Production of H 2 through the Transformation of Water on Pt/CeO 2 (111) and Pt/CeO x /TiO 2 (110) Catalysts journal, May 2012

Complexity in the Decomposition of Formic Acid on the TiO 2 (110) Surface journal, January 1997

Mechanistic study of low temperature CO2 methanation over Rh/TiO2 catalysts journal, May 2013

Advanced Electron Microscopy of Metal-Support Interactions in Supported Metal Catalysts journal, June 2011

The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts journal, April 2012

Imaging Cluster Surfaces with Atomic Resolution: The Strong Metal-Support Interaction State of Pt Supported on TiO 2 ( 110 ) journal, April 2000

Ship-in-bottle synthesis of anionic Rh carbonyls in faujasites journal, February 2001

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

Model catalyst studies of the strong metal–support interaction: Surface structure identified by STM on Pd nanoparticles on TiO2(110) journal, August 2005

Mean coordination numbers and the non-metal–metal transition in clusters journal, January 1992

Ceria Maintains Smaller Metal Catalyst Particles by Strong Metal-Support Bonding journal, August 2010

Strong metal-support interactions journal, November 1987

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Insight of the stability and activity of platinum single atoms on ceria journal, May 2019

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Pt Nanoparticles Supported over Porous Porphyrin Nanospheres for Chemoselective Hydrogenation Reactions journal, March 2019

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Direct 3D Printing of Reactive Agitating Impellers for the Convenient Treatment of Various Pollutants in Water journal, February 2018

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Designed Precursor for the Controlled Synthesis of Highly Active Atomic and Sub-nanometric Platinum Catalysts on Mesoporous Silica journal, March 2018

Interaction trends between single metal atoms and oxide supports identified with density functional theory and statistical learning journal, July 2018

Isolated Metal Active Site Concentration and Stability Control Catalytic CO ₂ Reduction Selectivity
journal, February 2015

Trends in the catalytic reduction of CO2 by hydrogen over supported monometallic and bimetallic catalysts
journal, May 2013

Counting electrons on supported nanoparticles
journal, December 2015

Zeolite-Supported Rhodium Complexes and Clusters: Switching Catalytic Selectivity by Controlling Structures of Essentially Molecular Species
journal, April 2011

Dynamic structural evolution of supported palladium–ceria core–shell catalysts revealed by in situ electron microscopy
journal, July 2015

SMSI effect in some reducible oxides including niobia
journal, April 1996

Catalytic reduction of CO ₂ by H ₂ for synthesis of CO, methanol and hydrocarbons: challenges and opportunities
journal, January 2016

Comparison of Metal-Support Interactions in Pt/TiO2 and Pt/CeO2
journal, August 1995

Real-space observation of strong metal-support interaction: state-of-the-art and what's the next: REAL-SPACE OBSERVATION OF STRONG METAL-SUPPORT INTERACTION
journal, December 2015

Effect of NO on the CO-induced disruption of rhodium crystallites
journal, July 1988

EXAFS evidence for direct metal-metal bonding in reduced rhodium/titania catalysts
journal, April 1986

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

Metal-Support Interactions in Rh/CeO2, Rh/TiO2, and Rh/Nb2O5 Catalysts as Inferred from CO2 Methanation Activity
journal, September 1995

Promotion of CO and CO2 Hydrogenation over Rh by Metal Oxides: The Influence of Oxide Lewis Acidity and Reducibility
journal, September 1994

An infrared study of the hydrogenation of carbon dioxide on supported rhodium catalysts
journal, April 1985

High-performance Ag–Co alloy catalysts for electrochemical oxygen reduction
journal, August 2014

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

In-situ FT-IR study on CO2 hydrogenation over Cu catalysts supported on SiO2, Al2O3, and TiO2
journal, December 1997

Dynamical Observation and Detailed Description of Catalysts under Strong Metal–Support Interaction
journal, June 2016

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
journal, January 1978

Multiple-scattering calculations of x-ray-absorption spectra
journal, July 1995

IFEFFIT : interactive XAFS analysis and FEFF fitting
journal, March 2001

Influence of Dipole–Dipole Interactions on Coverage-Dependent Adsorption: CO and NO on Pt(111)
journal, May 2012

Probing Terrace and Step Sites on Pt Nanoparticles Using CO and Ethylene
journal, April 2010

Magnetosomes could be protective shields against metal stress in magnetotactic bacteria
journal, July 2020

Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol
journal, March 2014

Finding optimal surface sites on heterogeneous catalysts by counting nearest neighbors
journal, October 2015

Engineering Selectivity in Heterogeneous Catalysis: Ag Nanowires as Selective Ethylene Epoxidation Catalysts
journal, August 2008

Charge Transfer in Metal Catalysts Supported on Doped TiO2: A Theoretical Approach Based on Metal–Semiconductor Contact Theory
journal, July 1996

Some contributions of electron microscopy to the characterisation of the strong metal–support interaction effect
journal, January 2003

Revealing particle growth mechanisms by combining high-surface-area catalysts made with monodisperse particles and electron microscopy conducted at atmospheric pressure
journal, May 2016

Selective methanation of CO over supported noble metal catalysts: Effects of the nature of the metallic phase on catalytic performance
journal, July 2008

Direct observation of the surfaces of small metal crystallites: rhodium supported on titania
journal, July 1988

The surface science of titanium dioxide
journal, January 2003

A versatile sample-environment cell for non-ambient X-ray scattering experiments
journal, July 2008

Mechanism of CO2 reduction by H2 on Ru(0 0 0 1) and general selectivity descriptors for late-transition metal catalysts
journal, November 2016

First-Principles Theoretical Study and Scanning Tunneling Microscopic Observation of Dehydration Process of Formic Acid on a TiO ₂ (110) Surface ^†
journal, September 2004

Metal-support effects on the intramolecular selectivity of crotonaldehyde hydrogenation over platinum
journal, January 1989

Electronic perturbations
journal, July 2012

A New Type of Strong Metal–Support Interaction and the Production of H ₂ through the Transformation of Water on Pt/CeO ₂ (111) and Pt/CeO _x /TiO ₂ (110) Catalysts
journal, May 2012

Complexity in the Decomposition of Formic Acid on the TiO ₂ (110) Surface
journal, January 1997

Mechanistic study of low temperature CO2 methanation over Rh/TiO2 catalysts
journal, May 2013

Advanced Electron Microscopy of Metal-Support Interactions in Supported Metal Catalysts
journal, June 2011

The Active Site of Methanol Synthesis over Cu/ZnO/Al₂O₃ Industrial Catalysts
journal, April 2012

Imaging Cluster Surfaces with Atomic Resolution: The Strong Metal-Support Interaction State of Pt Supported on ${TiO}_{2} (110)$
journal, April 2000

Ship-in-bottle synthesis of anionic Rh carbonyls in faujasites
journal, February 2001

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

Model catalyst studies of the strong metal–support interaction: Surface structure identified by STM on Pd nanoparticles on TiO2(110)
journal, August 2005

Mean coordination numbers and the non-metal–metal transition in clusters
journal, January 1992

Ceria Maintains Smaller Metal Catalyst Particles by Strong Metal-Support Bonding
journal, August 2010

Strong metal-support interactions
journal, November 1987

A redox interaction-engaged strategy for multicomponent nanomaterials
journal, January 2020

Regulating the size and spatial distribution of Pd nanoparticles supported by the defect engineered metal–organic framework HKUST-1 and applied in the aerobic oxidation of cinnamyl alcohol
journal, January 2019

Pulsed electric current boosts electrochemical performance and electro-conductivity of La _x Sr _{1− x} Cr _y Ni _{1− y} O ₃ perovskite via exsolution of nanoparticles
journal, August 2019

Recent advances in confining metal-based nanoparticles into carbon nanotubes for electrochemical energy conversion and storage devices
journal, January 2019

Defect engineering of metal–oxide interface for proximity of photooxidation and photoreduction
journal, May 2019

Catalytic Transfer Hydrogenation of Biomass‐Derived Substrates to Value‐Added Chemicals on Dual‐Function Catalysts: Opportunities and Challenges
journal, December 2018

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journal, November 2019

Understanding Heteroatom-Mediated Metal–Support Interactions in Functionalized Carbons: A Perspective Review
journal, July 2018

Hierarchically Porous Network-Like Ni/Co ₃ O ₄ : Noble Metal-Free Catalysts for Carbon Dioxide Methanation
journal, January 2018

Interface engineering of palladium and zinc oxide nanorods with strong metal–support interactions for enhanced hydrogen production from base-free formaldehyde solution
journal, January 2019

Activity enhancement of cobalt catalysts by tuning metal-support interactions
journal, October 2018

Enhancing electrostatic interactions to activate polar molecules: ammonia borane methanolysis on a Cu/Co(OH) ₂ nanohybrid
journal, January 2019

Insight of the stability and activity of platinum single atoms on ceria
journal, May 2019

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journal, March 2018

An Oxygen‐Vacancy‐Rich Semiconductor‐Supported Bifunctional Catalyst for Efficient and Stable Zinc–Air Batteries
journal, December 2018

Pt Nanoparticles Supported over Porous Porphyrin Nanospheres for Chemoselective Hydrogenation Reactions
journal, March 2019

Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal-Support Interaction
journal, August 2017

Heterogeneous single-atom catalysis
journal, May 2018

Classical strong metal–support interactions between gold nanoparticles and titanium dioxide
journal, October 2017

Recent Progress in Bifunctional Electrocatalysts for Overall Water Splitting under Acidic Conditions
journal, May 2019

Strong metal–support interaction improves activity and stability of Pt electrocatalysts on doped metal oxides
journal, January 2018

Tuning the Selectivity of Catalytic Carbon Dioxide Hydrogenation over Iridium/Cerium Oxide Catalysts with a Strong Metal-Support Interaction
journal, August 2017

Direct 3D Printing of Reactive Agitating Impellers for the Convenient Treatment of Various Pollutants in Water
journal, February 2018

Interfacial charge distributions in carbon-supported palladium catalysts
journal, August 2017

Designed Precursor for the Controlled Synthesis of Highly Active Atomic and Sub-nanometric Platinum Catalysts on Mesoporous Silica
journal, March 2018

Interaction trends between single metal atoms and oxide supports identified with density functional theory and statistical learning
journal, July 2018

Phase‐Dependent Stability and Substrate‐Induced Deactivation by Strong Metal‐Support Interaction of Ru/TiO ₂ Catalysts for the Hydrogenation of Levulinic Acid
journal, April 2019

Selective Hydrogenation of CO ₂ to Ethanol over Cobalt Catalysts
journal, April 2018

Cobalt nanoparticles mechanically deposited on α-Al ₂ O ₃ : a competitive catalyst for the production of hydrogen through ethanol steam reforming: Cobalt nanoparticles mechanically deposited on α-Al ₂ O ₃
journal, October 2018