Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction

Aitbekova, Aisulu; Wu, Liheng; Wrasman, Cody J.; Boubnov, Alexey; Hoffman, Adam S.; Goodman, Emmett D.; Bare, Simon R.; Cargnello, Matteo

doi:10.1021/jacs.8b07615

Title: Low-Temperature Restructuring of CeO₂-Supported Ru Nanoparticles Determines Selectivity in CO₂ Catalytic Reduction

Abstract

CO₂ reduction to higher value products is a promising way to produce fuels and key chemical building blocks while reducing CO₂ emissions. The reaction at atmospheric pressure mainly yields CH₄ via methanation and CO via the reverse water-gas shift (RWGS) reaction. Describing catalyst features that control the selectivity of these two pathways is important to determine the formation of specific products. At the same time, identification of morphological changes occurring to catalysts under reaction conditions can be crucial to tune their catalytic performance. In this contribution we investigate the dependency of selectivity for CO₂ reduction on the size of Ru nanoparticles (NPs) and on support. We find that even at rather low temperatures (210 °C), oxidative pretreatment induces redispersion of Ru NPs supported on CeO₂ and leads to a complete switch in the performance of this material from a well-known selective methanation catalyst to an active and selective RWGS catalyst. By utilizing in situ X-ray absorption spectroscopy, we demonstrate that the low-temperature redispersion process occurs via decomposition of the metal oxide phase with size-dependent kinetics, producing stable single-site RuO_x/CeO₂ species strongly bound to the CeO₂ support that are remarkably selective for CO production. Furthermore, these results show that reaction selectivitymore »« less

Authors:

Aitbekova, Aisulu ^[1]; Wu, Liheng ^[2]; Wrasman, Cody J. ^[1]; Boubnov, Alexey ^[3]; Hoffman, Adam S. ^[3]; Goodman, Emmett D. ^[1]; Bare, Simon R. ^[3];

^[1]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: 2018-09-25

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1484844

Grant/Contract Number:: AC02-76SF00515

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 140; Journal Issue: 42; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Aitbekova, Aisulu, Wu, Liheng, Wrasman, Cody J., Boubnov, Alexey, Hoffman, Adam S., Goodman, Emmett D., Bare, Simon R., and Cargnello, Matteo. Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction.  United States: N. p., 2018. 
Web.  doi:10.1021/jacs.8b07615.

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                    Aitbekova, Aisulu, Wu, Liheng, Wrasman, Cody J., Boubnov, Alexey, Hoffman, Adam S., Goodman, Emmett D., Bare, Simon R., & Cargnello, Matteo. Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction.  United States.  https://doi.org/10.1021/jacs.8b07615

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                    Aitbekova, Aisulu, Wu, Liheng, Wrasman, Cody J., Boubnov, Alexey, Hoffman, Adam S., Goodman, Emmett D., Bare, Simon R., and Cargnello, Matteo. Tue .  
"Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction".  United States.  https://doi.org/10.1021/jacs.8b07615.  https://www.osti.gov/servlets/purl/1484844.

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@article{osti_1484844,

  title        = {Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction},

  author       = {Aitbekova, Aisulu and Wu, Liheng and Wrasman, Cody J. and Boubnov, Alexey and Hoffman, Adam S. and Goodman, Emmett D. and Bare, Simon R. and Cargnello, Matteo},

  abstractNote = {CO2 reduction to higher value products is a promising way to produce fuels and key chemical building blocks while reducing CO2 emissions. The reaction at atmospheric pressure mainly yields CH4 via methanation and CO via the reverse water-gas shift (RWGS) reaction. Describing catalyst features that control the selectivity of these two pathways is important to determine the formation of specific products. At the same time, identification of morphological changes occurring to catalysts under reaction conditions can be crucial to tune their catalytic performance. In this contribution we investigate the dependency of selectivity for CO2 reduction on the size of Ru nanoparticles (NPs) and on support. We find that even at rather low temperatures (210 °C), oxidative pretreatment induces redispersion of Ru NPs supported on CeO2 and leads to a complete switch in the performance of this material from a well-known selective methanation catalyst to an active and selective RWGS catalyst. By utilizing in situ X-ray absorption spectroscopy, we demonstrate that the low-temperature redispersion process occurs via decomposition of the metal oxide phase with size-dependent kinetics, producing stable single-site RuOx/CeO2 species strongly bound to the CeO2 support that are remarkably selective for CO production. Furthermore, these results show that reaction selectivity can be heavily dependent on catalyst structure and that structural changes of the catalyst can occur even at low temperatures and can go unseen in materials with less defined structures.},

  doi          = {10.1021/jacs.8b07615},

  journal      = {Journal of the American Chemical Society},

  number       = 42,

  volume       = 140,

  place        = {United States},

  year         = {2018},

  month        = {9}

}

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Figure 1: Representative TEM images of the starting Ru NPs (a, 1.4 nm; b, 2.6 nm; c, 4.4 nm) and corresponding particle size distributions (d-f). (g-o) Samples utilized in this work: Ru/Al₂O₃ (g-i); Ru/TiO₂ (j-l); and Ru/CeO₂ (m-o) with increasing Ru particle size from top to bottom.

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https://doi.org/10.1016/0021-9517(94)90020-5

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Title: Low-Temperature Restructuring of CeO2-Supported Ru Nanoparticles Determines Selectivity in CO2 Catalytic Reduction

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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

Status and prospects in higher alcohols synthesis from syngas journal, January 2017

Tuning Selectivity of CO 2 Hydrogenation Reactions at the Metal/Oxide Interface journal, July 2017

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

Support effects in the formation of methanol from carbon dioxide and hydrogen over rhenium catalysts journal, January 1983

Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces journal, March 2011

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

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

CO 2 Reduction on Supported Ru/Al 2 O 3 Catalysts: Cluster Size Dependence of Product Selectivity journal, October 2013

A Temperature-Programmed and Transient Kinetic Study of CO2Activation and Methanation over CeO2Supported Noble Metals journal, February 1997

Recent advances in methanation catalysts for the production of synthetic natural gas journal, January 2015

Recent advances in catalytic hydrogenation of carbon dioxide journal, January 2011

Selective CO Methanation on Highly Active Ru/TiO 2 Catalysts: Identifying the Physical Origin of the Observed Activation/Deactivation and Loss in Selectivity journal, April 2018

Catalytic behavior of supported Ru nanoparticles on the {1 0 0}, {1 1 0}, and {1 1 1} facet of CeO2 journal, September 2015

Influence of the oxide support reducibility on the CO2 methanation over Ru-based catalysts journal, December 2017

Promotion of CO2 methanation activity and CH4 selectivity at low temperatures over Ru/CeO2/Al2O3 catalysts journal, June 2014

Low-Temperature CO 2 Methanation over CeO 2 -Supported Ru Single Atoms, Nanoclusters, and Nanoparticles Competitively Tuned by Strong Metal–Support Interactions and H-Spillover Effect journal, May 2018

Active Site Dependent Reaction Mechanism over Ru/CeO 2 Catalyst toward CO 2 Methanation journal, May 2016

CO2 methanation property of Ru nanoparticle-loaded TiO2 prepared by a polygonal barrel-sputtering method journal, January 2009

CO2 methanation on Ru-doped ceria journal, March 2011

CO 2 methanation by Ru-doped ceria: the role of the oxidation state of the surface journal, January 2015

Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts journal, September 2016

Metal Redispersion Strategies for Recycling of Supported Metal Catalysts: A Perspective journal, May 2015

Splitting of platinum crystallites supported on thin, nonporous alumina films journal, February 1976

Influence of oxidation-reduction treatment on dispersion of rhenium supported on γ-Al2O3 journal, November 1997

Room-Temperature Dynamics of Vanishing Copper Nanoparticles Supported on Silica journal, March 2017

Oxidation characteristics of Ru/CeO2 catalyst journal, July 2005

Intermolecular Coupling of Alkynes with Acrylates by Recyclable Oxide-Supported Ruthenium Catalysts: Formation of Distorted Ruthenium(IV)-oxo Species on Ceria as a Key Precursor of Active Species journal, October 2011

Ceria-supported ruthenium catalysts for the synthesis of indole via dehydrogenative N-heterocyclization journal, January 2011

Alkylamine Stabilized Ruthenium Nanocrystals: Faceting and Branching journal, July 2008

Efficient Removal of Organic Ligands from Supported Nanocrystals by Fast Thermal Annealing Enables Catalytic Studies on Well-Defined Active Phases journal, May 2015

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal, June 2005

Partial oxidation of methane over supported ruthenium catalysts journal, May 2007

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

Kinetic study on carbon dioxide hydrogenation over Ru/γ-Al2O3 catalysts journal, September 2008

Hydrogenation of CO2 to CH4 over alumina-supported noble metals journal, June 1980

Methanation of CO2 on supported rhodium catalyst journal, April 1981

Strong metal-support interactions in nickel/titania catalysts: The importance of interfacial phenomena journal, December 1982

Strong metal-support interactions journal, November 1987

Microstructural and Metal−Support Interactions of the Pt−CeO 2 /C Catalysts for Direct Methanol Fuel Cell Application journal, April 2011

Some recent results on metal/support interaction effects in NM/CeO2 (NM: noble metal) catalysts journal, April 1999

Rh–CeO 2 interaction induced by high-temperature reduction. Characterization and catalytic behaviour in transient and continuous conditions journal, January 1992

Promoting Effects of Hydrothermal Treatment on the Activity and Durability of Pd/CeO 2 Catalysts for CO Oxidation journal, September 2017

The State of Platinum in Re-Forming Catalysts journal, January 1963

Surface interactions in the system Re/$gamma;-Al2O3 journal, September 1976

Thermally stable single-atom platinum-on-ceria catalysts via atom trapping journal, July 2016

Tuning the Structure of Platinum Particles on Ceria In Situ for Enhancing the Catalytic Performance of Exhaust Gas Catalysts journal, September 2017

Dynamics and Thermodynamics of Pd–PdO Phase Transitions: Effects of Pd Cluster Size and Kinetic Implications for Catalytic Methane Combustion journal, January 2016

Polyhedral Shapes of CeO 2 Nanoparticles journal, December 2003

Synthesis of a ceria-supported iron–ruthenium oxide catalyst and its structural transformation from subnanometer clusters to single atoms during the Fischer–Tropsch synthesis reaction journal, January 2017

High-Performance Ru 1 /CeO 2 Single-Atom Catalyst for CO Oxidation: A Computational Exploration journal, August 2016

Towards advanced structural analysis of iron oxide clusters on the surface of γ-Al2O3 using EXAFS journal, November 2016

Selective CO 2 methanation on Ru/TiO 2 catalysts: unravelling the decisive role of the TiO 2 support crystal structure journal, January 2016

Thermolysis of Noble Metal Nanoparticles into Electron‐Rich Phosphorus‐Coordinated Noble Metal Single Atoms at Low Temperature journal, August 2019

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

Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO 2 Hydrogenation to Hydrocarbons journal, November 2019

Thermolysis of Noble Metal Nanoparticles into Electron‐Rich Phosphorus‐Coordinated Noble Metal Single Atoms at Low Temperature journal, August 2019

Influence of Coordination Environment of Anchored Single‐Site Cobalt Catalyst on CO 2 Hydrogenation journal, December 2019

Ultrafine Ag Nanoparticles as Active Catalyst for Electrocatalytic Hydrogen Production journal, October 2019

Silicon-doped graphene edges: an efficient metal-free catalyst for the reduction of CO 2 into methanol and ethanol journal, January 2019

A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO 2 reduction journal, January 2020

Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO 2 Hydrogenation to Hydrocarbons journal, November 2019

Title: Low-Temperature Restructuring of CeO₂-Supported Ru Nanoparticles Determines Selectivity in CO₂ Catalytic Reduction

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

Status and prospects in higher alcohols synthesis from syngas
journal, January 2017

Tuning Selectivity of CO ₂ Hydrogenation Reactions at the Metal/Oxide Interface
journal, July 2017

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

Support effects in the formation of methanol from carbon dioxide and hydrogen over rhenium catalysts
journal, January 1983

Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
journal, March 2011

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

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

CO ₂ Reduction on Supported Ru/Al ₂ O ₃ Catalysts: Cluster Size Dependence of Product Selectivity
journal, October 2013

A Temperature-Programmed and Transient Kinetic Study of CO2Activation and Methanation over CeO2Supported Noble Metals
journal, February 1997

Recent advances in methanation catalysts for the production of synthetic natural gas
journal, January 2015

Recent advances in catalytic hydrogenation of carbon dioxide
journal, January 2011

Selective CO Methanation on Highly Active Ru/TiO ₂ Catalysts: Identifying the Physical Origin of the Observed Activation/Deactivation and Loss in Selectivity
journal, April 2018

Catalytic behavior of supported Ru nanoparticles on the {1 0 0}, {1 1 0}, and {1 1 1} facet of CeO2
journal, September 2015

Influence of the oxide support reducibility on the CO2 methanation over Ru-based catalysts
journal, December 2017

Promotion of CO2 methanation activity and CH4 selectivity at low temperatures over Ru/CeO2/Al2O3 catalysts
journal, June 2014

Low-Temperature CO ₂ Methanation over CeO ₂ -Supported Ru Single Atoms, Nanoclusters, and Nanoparticles Competitively Tuned by Strong Metal–Support Interactions and H-Spillover Effect
journal, May 2018

Active Site Dependent Reaction Mechanism over Ru/CeO ₂ Catalyst toward CO ₂ Methanation
journal, May 2016

CO2 methanation property of Ru nanoparticle-loaded TiO2 prepared by a polygonal barrel-sputtering method
journal, January 2009

CO2 methanation on Ru-doped ceria
journal, March 2011

CO ₂ methanation by Ru-doped ceria: the role of the oxidation state of the surface
journal, January 2015

Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts
journal, September 2016

Metal Redispersion Strategies for Recycling of Supported Metal Catalysts: A Perspective
journal, May 2015

Splitting of platinum crystallites supported on thin, nonporous alumina films
journal, February 1976

Influence of oxidation-reduction treatment on dispersion of rhenium supported on γ-Al2O3
journal, November 1997

Room-Temperature Dynamics of Vanishing Copper Nanoparticles Supported on Silica
journal, March 2017

Oxidation characteristics of Ru/CeO2 catalyst
journal, July 2005

Intermolecular Coupling of Alkynes with Acrylates by Recyclable Oxide-Supported Ruthenium Catalysts: Formation of Distorted Ruthenium(IV)-oxo Species on Ceria as a Key Precursor of Active Species
journal, October 2011

Ceria-supported ruthenium catalysts for the synthesis of indole via dehydrogenative N-heterocyclization
journal, January 2011

Alkylamine Stabilized Ruthenium Nanocrystals: Faceting and Branching
journal, July 2008

Efficient Removal of Organic Ligands from Supported Nanocrystals by Fast Thermal Annealing Enables Catalytic Studies on Well-Defined Active Phases
journal, May 2015

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005

Partial oxidation of methane over supported ruthenium catalysts
journal, May 2007

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

Kinetic study on carbon dioxide hydrogenation over Ru/γ-Al2O3 catalysts
journal, September 2008

Hydrogenation of CO2 to CH4 over alumina-supported noble metals
journal, June 1980

Methanation of CO2 on supported rhodium catalyst
journal, April 1981

Strong metal-support interactions in nickel/titania catalysts: The importance of interfacial phenomena
journal, December 1982

Strong metal-support interactions
journal, November 1987

Microstructural and Metal−Support Interactions of the Pt−CeO ₂ /C Catalysts for Direct Methanol Fuel Cell Application
journal, April 2011

Some recent results on metal/support interaction effects in NM/CeO2 (NM: noble metal) catalysts
journal, April 1999

Rh–CeO ₂ interaction induced by high-temperature reduction. Characterization and catalytic behaviour in transient and continuous conditions
journal, January 1992

Promoting Effects of Hydrothermal Treatment on the Activity and Durability of Pd/CeO ₂ Catalysts for CO Oxidation
journal, September 2017

The State of Platinum in Re-Forming Catalysts
journal, January 1963

Surface interactions in the system Re/$gamma;-Al2O3
journal, September 1976

Thermally stable single-atom platinum-on-ceria catalysts via atom trapping
journal, July 2016

Tuning the Structure of Platinum Particles on Ceria In Situ for Enhancing the Catalytic Performance of Exhaust Gas Catalysts
journal, September 2017

Dynamics and Thermodynamics of Pd–PdO Phase Transitions: Effects of Pd Cluster Size and Kinetic Implications for Catalytic Methane Combustion
journal, January 2016

Polyhedral Shapes of CeO ₂ Nanoparticles
journal, December 2003

Synthesis of a ceria-supported iron–ruthenium oxide catalyst and its structural transformation from subnanometer clusters to single atoms during the Fischer–Tropsch synthesis reaction
journal, January 2017

High-Performance Ru ₁ /CeO ₂ Single-Atom Catalyst for CO Oxidation: A Computational Exploration
journal, August 2016

Towards advanced structural analysis of iron oxide clusters on the surface of γ-Al2O3 using EXAFS
journal, November 2016

Selective CO ₂ methanation on Ru/TiO ₂ catalysts: unravelling the decisive role of the TiO ₂ support crystal structure
journal, January 2016

Thermolysis of Noble Metal Nanoparticles into Electron‐Rich Phosphorus‐Coordinated Noble Metal Single Atoms at Low Temperature
journal, August 2019

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

Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO ₂ Hydrogenation to Hydrocarbons
journal, November 2019

Thermolysis of Noble Metal Nanoparticles into Electron‐Rich Phosphorus‐Coordinated Noble Metal Single Atoms at Low Temperature
journal, August 2019

Influence of Coordination Environment of Anchored Single‐Site Cobalt Catalyst on CO ₂ Hydrogenation
journal, December 2019

Ultrafine Ag Nanoparticles as Active Catalyst for Electrocatalytic Hydrogen Production
journal, October 2019

Silicon-doped graphene edges: an efficient metal-free catalyst for the reduction of CO ₂ into methanol and ethanol
journal, January 2019

A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO ₂ reduction
journal, January 2020

Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO ₂ Hydrogenation to Hydrocarbons
journal, November 2019