Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions

Wang, Hui; Dong, Jinshi; Allard, Lawrence F.; Lee, Sungsik; Oh, Se; Wang, Jun; Li, Wei; Shen, Meiqing; Yang, Ming

doi:10.1016/j.apcatb.2018.11.034

Title: Single-site Pt/La-Al₂O₃ stabilized by barium as an active and stable catalyst in purifying CO and C₃H₆ emissions

Abstract

High-temperature operations present a substantial challenge for developing industrial-capable precious metal catalysts (e.g. Pt/alumina), where the scarce metal atoms easily become wasted as sintered nanoparticles. Using fully dispersed precious metal atoms to deliver the catalysis remains an elusive goal. On a widely used La-stabilized alumina support, we find that the atomically dispersed Pt₁(II)-O_x- species, rather than the much more visible large metal particles, are the actual catalytic sites for the CO and C₃H₆ oxidation reactions. Unfortunately, the La dopants in alumina support will not hinder the sintering of the active Pt1(II)-Ox- species. As a natural next step, the Ba-Ox- species were introduced to specifically stabilize the single-atom Pt on the La-stabilized alumina support. By implementing this improved formulation, the atomically dispersed Pt on alumina retains the original full dispersion even after 650 °C hydrothermal aging. Intriguingly, with or without the barium additives and/or sintered platinum particles in the catalysts, the intrinsic activity per Pt atom stays intact. Along with other experimental evidence, this leads to the finding that the single-atom Pt is the true catalytic site for the oxidation of CO and C₃H₆ in the widely-used Pt/La-Al₂O₃ material system. This work provides a new perspective for efficient precious metal utilizationmore » under demanding catalytic conditions.« less

Authors:

Wang, Hui ^[1]; Dong, Jinshi ^[1]; Allard, Lawrence F. ^[2]; Lee, Sungsik ^[3]; Oh, Se ^[4]; Wang, Jun ^[1]; Li, Wei ^[4]; Shen, Meiqing ^[1]; Yang, Ming ^[4]

Tianjin Univ., Tianjin (China). School of Chemical Engineering & Technology
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
General Motors Global Research and Development, Warren, MI (United States). Chemical and Materials Systems Lab.

Publication Date:: Mon Nov 19 00:00:00 EST 2018

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); General Motors, R&D, Warren, MI (United States); National Key Research and Development Program of China

OSTI Identifier:: 1492696

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Applied Catalysis B: Environmental

Additional Journal Information:: Journal Volume: 244; Journal Issue: C; Journal ID: ISSN 0926-3373

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Alumina; Emissions purification; High-temperature stability; Platinum; Single-atom catalyst

Citation Formats


                    Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, and Yang, Ming. Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions.  United States: N. p., 2018. 
Web.  doi:10.1016/j.apcatb.2018.11.034.

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                    Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, & Yang, Ming. Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions.  United States.  https://doi.org/10.1016/j.apcatb.2018.11.034

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                    Wang, Hui, Dong, Jinshi, Allard, Lawrence F., Lee, Sungsik, Oh, Se, Wang, Jun, Li, Wei, Shen, Meiqing, and Yang, Ming. Mon .  
"Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions".  United States.  https://doi.org/10.1016/j.apcatb.2018.11.034.  https://www.osti.gov/servlets/purl/1492696.

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@article{osti_1492696,

  title        = {Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions},

  author       = {Wang, Hui and Dong, Jinshi and Allard, Lawrence F. and Lee, Sungsik and Oh, Se and Wang, Jun and Li, Wei and Shen, Meiqing and Yang, Ming},

  abstractNote = {High-temperature operations present a substantial challenge for developing industrial-capable precious metal catalysts (e.g. Pt/alumina), where the scarce metal atoms easily become wasted as sintered nanoparticles. Using fully dispersed precious metal atoms to deliver the catalysis remains an elusive goal. On a widely used La-stabilized alumina support, we find that the atomically dispersed Pt1(II)-Ox- species, rather than the much more visible large metal particles, are the actual catalytic sites for the CO and C3H6 oxidation reactions. Unfortunately, the La dopants in alumina support will not hinder the sintering of the active Pt1(II)-Ox- species. As a natural next step, the Ba-Ox- species were introduced to specifically stabilize the single-atom Pt on the La-stabilized alumina support. By implementing this improved formulation, the atomically dispersed Pt on alumina retains the original full dispersion even after 650 °C hydrothermal aging. Intriguingly, with or without the barium additives and/or sintered platinum particles in the catalysts, the intrinsic activity per Pt atom stays intact. Along with other experimental evidence, this leads to the finding that the single-atom Pt is the true catalytic site for the oxidation of CO and C3H6 in the widely-used Pt/La-Al2O3 material system. This work provides a new perspective for efficient precious metal utilization under demanding catalytic conditions.},

  doi          = {10.1016/j.apcatb.2018.11.034},

  journal      = {Applied Catalysis B: Environmental},

  number       = C,

  volume       = 244,

  place        = {United States},

  year         = {Mon Nov 19 00:00:00 EST 2018},

  month        = {Mon Nov 19 00:00:00 EST 2018}

}

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Transmission electron microscopy and energy dispersive x-ray spectroscopy studies of Pt-Re/[gamma]-Al[sub 2]O[sub 3] catalysts

Journal Article Huang, Z ; Fryer, J R ; Park, C ; ... - Journal of Catalysis; (United States)

A series of Pt/[gamma]-Al[sub 2]O[sub 3], Re/[gamma]-Al[sub 2]O[sub 3], and Pt-Re/[gamma]-Al-O[sub 3] catalysts have been studied by transmission electron microscopy and energy dispersive X-ray spectroscopy. It has been shown that rhenium was not alloyed with platinum, but widely dispersed on the surface of alumina. Two types of platinum were found: (i) three-dimensional metallic particles, and (ii) small particles consisting of a few platinum atoms. Some aggregation of the platinum particles occurred during use of the catalysts in the reforming of octane. It is suggested that the interaction of rhenium with the alumina support and therefore the modification to the platinummore »« less
https://doi.org/10.1006/jcat.1994.1234

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Title: Single-site Pt/La-Al2O3 stabilized by barium as an active and stable catalyst in purifying CO and C3H6 emissions

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Atomically Dispersed Au–(OH) x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction journal, March 2013

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A Single-Site Platinum CO Oxidation Catalyst in Zeolite KLTL: Microscopic and Spectroscopic Determination of the Locations of the Platinum Atoms journal, July 2014

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Remarkable NO oxidation on single supported platinum atoms journal, November 2014

Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts journal, August 2003

In Situ Redispersion of Platinum Autoexhaust Catalysts: An On-Line Approach to Increasing Catalyst Lifetimes? journal, October 2008

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Role of the Ceria–Zirconia Support in the Reactivity of Platinum and Palladium Catalysts for Methane Total Oxidation under Lean Conditions journal, October 2001

Pd/Support Interface-Promoted Pd−Ce 0.7 Zr 0.3 O 2 −Al 2 O 3 Automobile Three-Way Catalysts: Studying the Dynamic Oxygen Storage Capacity and CO, C 3 H 8 , and NO Conversion journal, February 2009

Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts journal, September 2015

Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation journal, July 2017

Effect of sintering on the catalytic activity of a Pt based catalyst for CO oxidation: Experiments and modeling journal, September 2008

Effect of Particle Morphology on the Ripening of Supported Pt Nanoparticles journal, February 2012

Correlation between catalytic activity and catalytic surface area of a Pt/Al2O3 DOC: An experimental and microkinetic modeling study journal, September 2014

Role of Pentacoordinated Al 3+ Ions in the High Temperature Phase Transformation of γ-Al 2 O 3 journal, May 2008

Renewable H2 from Glycerol Steam Reforming: Effect of La2O3 and CeO2 Addition to Pt/Al2O3 catalysts. journal, April 2010

Catalytic behavior of potassium containing compounds for diesel soot combustion journal, January 2006

Hard and Soft Acids and Bases journal, November 1963

Acids and Bases journal, January 1966

Pt-Ba/alumina NOx storage-reduction catalysts: Influence of Ba loading on NOx storage behavior journal, October 2005

Simultaneous removal of NOx and soot on Pt–Ba/Al2O3 NSR catalysts journal, April 2006

Pt dispersion effects during NOx storage and reduction on Pt/BaO/Al2O3 catalysts journal, August 2009

Sintering of Pt Nanoparticles via Volatile PtO 2 : Simulation and Comparison with Experiments journal, September 2016

Surface area stability and characterisation of a novel sulfate-based alumina modified by rare earth and alkaline earth ions journal, January 1994

Influence of reductant on the thermal stability of stored NOx in Pt/Ba/Al2O3 NOx storage and reduction traps journal, May 2004

Mesoporous silica–alumina modified by acid leaching as support of Pt catalysts in HDS of model compounds journal, October 2010

Strontium-Doped Perovskites Rival Platinum Catalysts for Treating NOx in Simulated Diesel Exhaust journal, March 2010

CO Oxidation on Metal Oxide Supported Single Pt atoms: The Role of the Support journal, June 2017

Chemisorption of CO and Mechanism of CO Oxidation on Supported Platinum Nanoclusters journal, March 2011

Effect of hydrothermal aging on oxygen storage/release and activity in a commercial automotive catalyst journal, July 1995

Reaction Kinetics of C3H6 Oxidation for Various Reaction Pathways Over Diesel Oxidation Catalysts journal, July 2013

Mechanisms of CO oxidation reaction and effect of chlorine ions on the CO oxidation reaction over Pt/CeO2 and Pt/CeO2/γ-Al2O3 catalysts journal, December 2004

FT-IR study of CO adsorption on Pt/CeO2: characterisation and structural rearrangement of small Pt particles journal, January 2005

Infrared studies of CO oxidation by oxygen and by water over Pt/Al2O3 and Pd/Al2O3 catalysts journal, February 2012

Improved Low-Temperature CO Oxidation Performance of Pd Supported on La-Stabilized Alumina journal, April 2013

The effect of steam and hydrogen in promoting the oxidation of carbon monoxide over a platinum on alumina catalyst journal, January 1991

Kinetic Study of the CO Oxidation over Pt/γ-Al2O3and Pt/Rh/CeO2/γ-Al2O3in the Presence of H2O and CO2 journal, October 1997

Reduction of Low Temperature Engine Pollutants by Understanding the Exhaust Species Interactions in a Diesel Oxidation Catalyst journal, January 2014

Modeling of two-step CO oxidation light-off on Pt/γ-Al2O3 in the presence of C3H6 and NO journal, October 2018

Understanding the nature of surface nitrates in BaO/γ-Al2O3 NOx storage materials: A combined experimental and theoretical study journal, January 2009

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Catalyst Architecture for Stable Single Atom Dispersion Enables Site-Specific Spectroscopic and Reactivity Measurements of CO Adsorbed to Pt Atoms, Oxidized Pt Clusters, and Metallic Pt Clusters on TiO 2 journal, September 2017

Beating Heterogeneity of Single-Site Catalysts: MgO-Supported Iridium Complexes journal, March 2018

Activation of surface lattice oxygen in single-atom Pt/CeO 2 for low-temperature CO oxidation journal, December 2017

The effect of gold particle size on AuAu bond length and reactivity toward oxygen in supported catalysts journal, June 2006

Strong Local Coordination Structure Effects on Subnanometer PtO x Clusters over CeO 2 Nanowires Probed by Low-Temperature CO Oxidation journal, August 2015

CO Oxidation on Supported Single Pt Atoms: Experimental and ab Initio Density Functional Studies of CO Interaction with Pt Atom on θ-Al 2 O 3 (010) Surface journal, August 2013

Structure–activity relationships of Pt/Al2O3 catalysts for CO and NO oxidation at diesel exhaust conditions journal, September 2012

The Effect of Pt Particle Size on the Oxidation of CO, C3H6, and NO Over Pt/Al2O3 for Diesel Exhaust Aftertreatment journal, June 2017

Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts journal, July 2013

Size and Support Effects for the Water–Gas Shift Catalysis over Gold Nanoparticles Supported on Model Al 2 O 3 and TiO 2 journal, February 2012

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

Active Oxygen on a Au/TiO2 Catalyst: Formation, Stability, and CO Oxidation Activity journal, July 2011

Surface chemistry models of carbon monoxide oxidation on supported platinum catalysts journal, October 1980

Utilizing Quantitative in Situ FTIR Spectroscopy To Identify Well-Coordinated Pt Atoms as the Active Site for CO Oxidation on Al 2 O 3 -Supported Pt Catalysts journal, July 2016

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Title: Single-site Pt/La-Al₂O₃ stabilized by barium as an active and stable catalyst in purifying CO and C₃H₆ emissions

Atomically Dispersed Supported Metal Catalysts
journal, July 2012

Tens of thousands of atoms replaced by one
journal, September 2015

Alkali-Stabilized Pt-OHx Species Catalyze Low-Temperature Water-Gas Shift Reactions
journal, September 2010

Atomically Dispersed Au–(OH) _x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction
journal, March 2013

Catalytically active Au-O(OH) _x - species stabilized by alkali ions on zeolites and mesoporous oxides
journal, November 2014

A Common Single-Site Pt(II)–O(OH) _x – Species Stabilized by Sodium on “Active” and “Inert” Supports Catalyzes the Water-Gas Shift Reaction
journal, March 2015

A Single-Site Platinum CO Oxidation Catalyst in Zeolite KLTL: Microscopic and Spectroscopic Determination of the Locations of the Platinum Atoms
journal, July 2014

Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011

Low-temperature carbon monoxide oxidation catalysed by regenerable atomically dispersed palladium on alumina
journal, September 2014

Remarkable NO oxidation on single supported platinum atoms
journal, November 2014

Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts
journal, August 2003

In Situ Redispersion of Platinum Autoexhaust Catalysts: An On-Line Approach to Increasing Catalyst Lifetimes?
journal, October 2008

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

Role of the Ceria–Zirconia Support in the Reactivity of Platinum and Palladium Catalysts for Methane Total Oxidation under Lean Conditions
journal, October 2001

Pd/Support Interface-Promoted Pd−Ce _0.7 Zr _0.3 O ₂ −Al ₂ O ₃ Automobile Three-Way Catalysts: Studying the Dynamic Oxygen Storage Capacity and CO, C ₃ H ₈ , and NO Conversion
journal, February 2009

Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
journal, September 2015

Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation
journal, July 2017

Effect of sintering on the catalytic activity of a Pt based catalyst for CO oxidation: Experiments and modeling
journal, September 2008

Effect of Particle Morphology on the Ripening of Supported Pt Nanoparticles
journal, February 2012

Correlation between catalytic activity and catalytic surface area of a Pt/Al2O3 DOC: An experimental and microkinetic modeling study
journal, September 2014

Role of Pentacoordinated Al ³⁺ Ions in the High Temperature Phase Transformation of γ-Al ₂ O ₃
journal, May 2008

Renewable H2 from Glycerol Steam Reforming: Effect of La2O3 and CeO2 Addition to Pt/Al2O3 catalysts.
journal, April 2010

Catalytic behavior of potassium containing compounds for diesel soot combustion
journal, January 2006

Hard and Soft Acids and Bases
journal, November 1963

Acids and Bases
journal, January 1966

Pt-Ba/alumina NOx storage-reduction catalysts: Influence of Ba loading on NOx storage behavior
journal, October 2005

Simultaneous removal of NOx and soot on Pt–Ba/Al2O3 NSR catalysts
journal, April 2006

Pt dispersion effects during NOx storage and reduction on Pt/BaO/Al2O3 catalysts
journal, August 2009

Sintering of Pt Nanoparticles via Volatile PtO ₂ : Simulation and Comparison with Experiments
journal, September 2016

Surface area stability and characterisation of a novel sulfate-based alumina modified by rare earth and alkaline earth ions
journal, January 1994

Influence of reductant on the thermal stability of stored NOx in Pt/Ba/Al2O3 NOx storage and reduction traps
journal, May 2004

Mesoporous silica–alumina modified by acid leaching as support of Pt catalysts in HDS of model compounds
journal, October 2010

Strontium-Doped Perovskites Rival Platinum Catalysts for Treating NO_x in Simulated Diesel Exhaust
journal, March 2010

CO Oxidation on Metal Oxide Supported Single Pt atoms: The Role of the Support
journal, June 2017

Chemisorption of CO and Mechanism of CO Oxidation on Supported Platinum Nanoclusters
journal, March 2011

Effect of hydrothermal aging on oxygen storage/release and activity in a commercial automotive catalyst
journal, July 1995

Reaction Kinetics of C3H6 Oxidation for Various Reaction Pathways Over Diesel Oxidation Catalysts
journal, July 2013

Mechanisms of CO oxidation reaction and effect of chlorine ions on the CO oxidation reaction over Pt/CeO2 and Pt/CeO2/γ-Al2O3 catalysts
journal, December 2004

FT-IR study of CO adsorption on Pt/CeO2: characterisation and structural rearrangement of small Pt particles
journal, January 2005

Infrared studies of CO oxidation by oxygen and by water over Pt/Al2O3 and Pd/Al2O3 catalysts
journal, February 2012

Improved Low-Temperature CO Oxidation Performance of Pd Supported on La-Stabilized Alumina
journal, April 2013

The effect of steam and hydrogen in promoting the oxidation of carbon monoxide over a platinum on alumina catalyst
journal, January 1991

Kinetic Study of the CO Oxidation over Pt/γ-Al2O3and Pt/Rh/CeO2/γ-Al2O3in the Presence of H2O and CO2
journal, October 1997

Reduction of Low Temperature Engine Pollutants by Understanding the Exhaust Species Interactions in a Diesel Oxidation Catalyst
journal, January 2014

Modeling of two-step CO oxidation light-off on Pt/γ-Al2O3 in the presence of C3H6 and NO
journal, October 2018

Understanding the nature of surface nitrates in BaO/γ-Al2O3 NOx storage materials: A combined experimental and theoretical study
journal, January 2009

Formation of featured nano-structure in thermal stable La-doped alumina composite catalyst
journal, December 2009

Relation between Crystallite Size and Dispersion on Supported Metal Catalysts
journal, October 1997

Catalyst Architecture for Stable Single Atom Dispersion Enables Site-Specific Spectroscopic and Reactivity Measurements of CO Adsorbed to Pt Atoms, Oxidized Pt Clusters, and Metallic Pt Clusters on TiO ₂
journal, September 2017

Beating Heterogeneity of Single-Site Catalysts: MgO-Supported Iridium Complexes
journal, March 2018

Activation of surface lattice oxygen in single-atom Pt/CeO ₂ for low-temperature CO oxidation
journal, December 2017

The effect of gold particle size on AuAu bond length and reactivity toward oxygen in supported catalysts
journal, June 2006

Strong Local Coordination Structure Effects on Subnanometer PtO _x Clusters over CeO ₂ Nanowires Probed by Low-Temperature CO Oxidation
journal, August 2015

CO Oxidation on Supported Single Pt Atoms: Experimental and ab Initio Density Functional Studies of CO Interaction with Pt Atom on θ-Al ₂ O ₃ (010) Surface
journal, August 2013

Structure–activity relationships of Pt/Al2O3 catalysts for CO and NO oxidation at diesel exhaust conditions
journal, September 2012

The Effect of Pt Particle Size on the Oxidation of CO, C3H6, and NO Over Pt/Al2O3 for Diesel Exhaust Aftertreatment
journal, June 2017

Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts
journal, July 2013

Size and Support Effects for the Water–Gas Shift Catalysis over Gold Nanoparticles Supported on Model Al ₂ O ₃ and TiO ₂
journal, February 2012

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

Active Oxygen on a Au/TiO2 Catalyst: Formation, Stability, and CO Oxidation Activity
journal, July 2011

Surface chemistry models of carbon monoxide oxidation on supported platinum catalysts
journal, October 1980

Utilizing Quantitative in Situ FTIR Spectroscopy To Identify Well-Coordinated Pt Atoms as the Active Site for CO Oxidation on Al ₂ O ₃ -Supported Pt Catalysts
journal, July 2016

Surpassing the single-atom catalytic activity limit through paired Pt-O-Pt ensemble built from isolated Pt1 atoms
journal, August 2019