Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons

Zhang, Pengfei; Lu, Hanfeng; Zhou, Ying; Zhang, Li; Wu, Zili; Yang, Shize; Shi, Hongliang; Zhu, Qiulian; Chen, Yinfei; Dai, Sheng

doi:10.1038/ncomms9446

Title: Mesoporous MnCeO_x solid solutions for low temperature and selective oxidation of hydrocarbons

Abstract

The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C–H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn_0.5Ce_0.5O_x solid solution that is highly active for the selective oxidation of hydrocarbons under mild conditions (100–120 °C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/cyclohexanol (100 °C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140–160 °C, conversion: 3-5%). Finally, the high activity can be attributed to the formation of a Mn_0.5Ce_0.5O_x solid solution with an ultrahigh manganese doping concentration in the CeO₂ cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C–H bonds and highly reducible Mn⁴⁺ ions for the rapid migration of oxygen vacancies from the bulk to the surface.

Authors:

Zhang, Pengfei ^[1]; Lu, Hanfeng ^[2]; Zhou, Ying ^[2]; Zhang, Li ^[1]; Wu, Zili ^[1]; Yang, Shize ^[1]; Shi, Hongliang ^[1]; Zhu, Qiulian ^[2]; Chen, Yinfei ^[2]; Dai, Sheng ^[3]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Zhejiang Univ. of Technology, Hangzhou (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: Thu Oct 15 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

OSTI Identifier:: 1259683

Grant/Contract Number:: 21107096; 21506194; LY14E080008; 2013C03021

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 6; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

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

Citation Formats


                    Zhang, Pengfei, Lu, Hanfeng, Zhou, Ying, Zhang, Li, Wu, Zili, Yang, Shize, Shi, Hongliang, Zhu, Qiulian, Chen, Yinfei, and Dai, Sheng. Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons.  United States: N. p., 2015. 
Web.  doi:10.1038/ncomms9446.

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                    Zhang, Pengfei, Lu, Hanfeng, Zhou, Ying, Zhang, Li, Wu, Zili, Yang, Shize, Shi, Hongliang, Zhu, Qiulian, Chen, Yinfei, & Dai, Sheng. Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons.  United States.  https://doi.org/10.1038/ncomms9446

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                    Zhang, Pengfei, Lu, Hanfeng, Zhou, Ying, Zhang, Li, Wu, Zili, Yang, Shize, Shi, Hongliang, Zhu, Qiulian, Chen, Yinfei, and Dai, Sheng. Thu .  
"Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons".  United States.  https://doi.org/10.1038/ncomms9446.  https://www.osti.gov/servlets/purl/1259683.

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@article{osti_1259683,

  title        = {Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons},

  author       = {Zhang, Pengfei and Lu, Hanfeng and Zhou, Ying and Zhang, Li and Wu, Zili and Yang, Shize and Shi, Hongliang and Zhu, Qiulian and Chen, Yinfei and Dai, Sheng},

  abstractNote = {The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C–H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn0.5Ce0.5Ox solid solution that is highly active for the selective oxidation of hydrocarbons under mild conditions (100–120 °C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/cyclohexanol (100 °C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140–160 °C, conversion: 3-5%). Finally, the high activity can be attributed to the formation of a Mn0.5Ce0.5Ox solid solution with an ultrahigh manganese doping concentration in the CeO2 cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C–H bonds and highly reducible Mn4+ ions for the rapid migration of oxygen vacancies from the bulk to the surface.},

  doi          = {10.1038/ncomms9446},

  journal      = {Nature Communications},

  number       = ,

  volume       = 6,

  place        = {United States},

  year         = {Thu Oct 15 00:00:00 EDT 2015},

  month        = {Thu Oct 15 00:00:00 EDT 2015}

}

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Title: Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons

Abstract

Citation Formats

Green, Catalytic Oxidation of Alcohols in Water journal, March 2000

Solvent-Free Oxidation of Primary Alcohols to Aldehydes Using Au-Pd/TiO 2 Catalysts journal, January 2006

Free Radical Functionalization of Organic Compounds Catalyzed by N- Hydroxyphthalimide † journal, September 2007

Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity journal, August 2013

Mesoporous Co 3 O 4 and Au/Co 3 O 4 Catalysts for Low-Temperature Oxidation of Trace Ethylene journal, March 2010

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CHEMISTRY: Palladium-Catalyzed Oxidation of Organic Chemicals with O2 journal, September 2005

A data-intensive approach to mechanistic elucidation applied to chiral anion catalysis journal, February 2015

Solvent-Free Oxidation of Primary Carbon-Hydrogen Bonds in Toluene Using Au-Pd Alloy Nanoparticles journal, January 2011

Overcoming the limitations of directed C–H functionalizations of heterocycles journal, November 2014

Interfacial Effects in Iron-Nickel Hydroxide-Platinum Nanoparticles Enhance Catalytic Oxidation journal, May 2014

Tuning Selectivity in Propylene Epoxidation by Plasmon Mediated Photo-Switching of Cu Oxidation State journal, March 2013

Adding Aliphatic C-H Bond Oxidations to Synthesis journal, February 2012

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Reactivity of the Gold/Water Interface During Selective Oxidation Catalysis journal, September 2010

CHEMISTRY: Selective Hydrocarbon Oxidation in Zeolites journal, July 2006

Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst journal, June 2006

Highly Selective Liquid-Phase Oxidation of Cyclohexane to KA Oil over Ti-MWW Catalyst: Evidence of Formation of Oxyl Radicals journal, December 2013

Alkane Oxidation with Molecular Oxygen Using a New Efficient Catalytic System: N -Hydroxyphthalimide (NHPI) Combined with Co(acac) n ( n = 2 or 3) † journal, January 1996

Effective catalysis of simple metalloporphyrins for cyclohexane oxidation with air in the absence of additives and solvents journal, June 2003

Designing a Heterogeneous Catalyst for the Production of Adipic Acid by Aerial Oxidation of Cyclohexane journal, July 2000

Aerobic Oxidation of Cyclohexane Catalyzed by Size-Controlled Au Clusters on Hydroxyapatite: Size Effect in the Sub-2 nm Regime journal, December 2010

Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions journal, October 2005

Selective oxidation with dioxygen by gold nanoparticle catalysts derived from 55-atom clusters journal, August 2008

Metal-Free Activation of Dioxygen by Graphene/g-C 3 N 4 Nanocomposites: Functional Dyads for Selective Oxidation of Saturated Hydrocarbons journal, June 2011

Selective Catalysis of the Aerobic Oxidation of Cyclohexane in the Liquid Phase by Carbon Nanotubes journal, March 2011

Recent Advances in Manganese Oxide Nanocrystals: Fabrication, Characterization, and Microstructure journal, March 2012

MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures journal, July 2004

Nanostructured manganese doped ceria solid solutions for CO oxidation at lower temperatures journal, January 2015

VOC oxidation over MnOx–CeO2 catalysts prepared by a combustion method journal, October 2008

A theoretic insight into the catalytic activity promotion of CeO2 surfaces by Mn doping journal, January 2012

Catalytic combustion of chlorobenzene over MnOx–CeO2 mixed oxide catalysts journal, February 2009

Surfactant-Assisted Synthesis, Characterizations, and Catalytic Oxidation Mechanisms of the Mesoporous MnOx−CeO 2 and Pd/MnOx−CeO 2 Catalysts Used for CO and C 3 H 8 Oxidation journal, November 2009

Catalytic removal of benzene over CeO2–MnOx composite oxides prepared by hydrothermal method journal, July 2013

Structure, Bonding, and Catalytic Activity of Monodisperse, Transition-Metal-Substituted CeO 2 Nanoparticles journal, November 2014

“Host−Guest” Chemistry in the Synthesis of Ordered Nonsiliceous Mesoporous Materials journal, July 2006

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Unique Spatial Heterogeneity in Ionic Liquids journal, September 2005

A general approach to crystalline and monomodal pore size mesoporous materials journal, December 2013

Updating Biomass into Functional Carbon Material in Ionothermal Manner journal, July 2014

The chemical nature of the C–H⊕⋯X− (X=Cl or Br) interaction in imidazolium halide ionic liquids journal, January 2006

The Structure of a Room-Temperature Ionic Liquid with and without Trace Amounts of Water: The Role of CH⋅⋅⋅O and CH⋅⋅⋅F Interactions in 1-n-Butyl-3-Methylimidazolium Tetrafluoroborate journal, September 2003

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Metal organic frameworks (MOFs) as catalysts: A combination of Cu2+ and Co2+ MOFs as an efficient catalyst for tetralin oxidation journal, April 2008

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Recent Advances in Transition Metal Catalyzed Oxidation of Organic Substrates with Molecular Oxygen journal, October 2005

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“Host—Guest” Chemistry in the Synthesis of Ordered Nonsiliceous Mesoporous Materials journal, October 2006

Selective Catalysis of the Aerobic Oxidation of Cyclohexane in the Liquid Phase by Carbon Nanotubes journal, March 2011

Free Radical Functionalization of Organic Compounds Catalyzed by N-Hydroxyphthalimide journal, December 2007

VOC oxidation over MnOx–CeO2 catalysts prepared by a combustion method journal, October 2008

Updating Biomass into Functional Carbon Material in Ionothermal Manner journal, July 2014

Recent Advances in Transition Metal Catalyzed Oxidation of Organic Substrates with Molecular Oxygen journal, June 2005

Recent Advances in Manganese Oxide Nanocrystals: Fabrication, Characterization, and Microstructure journal, March 2012

Unique Spatial Heterogeneity in Ionic Liquids journal, September 2005

Metal-Free Activation of Dioxygen by Graphene/g-C 3 N 4 Nanocomposites: Functional Dyads for Selective Oxidation of Saturated Hydrocarbons journal, June 2011

Mesoporous Co 3 O 4 and Au/Co 3 O 4 Catalysts for Low-Temperature Oxidation of Trace Ethylene journal, March 2010

Metal-free oxidation of aromatic carbon–hydrogen bonds through a reverse-rebound mechanism journal, July 2013

Overcoming the limitations of directed C–H functionalizations of heterocycles journal, November 2014

Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity journal, August 2013

Efficient stereo- and regioselective hydroxylation of alkanes catalysed by a bulky polyoxometalate journal, May 2010

A general approach to crystalline and monomodal pore size mesoporous materials journal, December 2013

Reactivity of the Gold/Water Interface During Selective Oxidation Catalysis journal, September 2010

Solvent-Free Oxidation of Primary Carbon-Hydrogen Bonds in Toluene Using Au-Pd Alloy Nanoparticles journal, January 2011

Interfacial Effects in Iron-Nickel Hydroxide-Platinum Nanoparticles Enhance Catalytic Oxidation journal, May 2014

Green, Catalytic Oxidation of Alcohols in Water journal, March 2000

Mixed‐Valence Single‐Atom Catalyst Derived from Functionalized Graphene journal, February 2019

Asymmetric Oxygen Vacancies: the Intrinsic Redox Active Sites in Metal Oxide Catalysts journal, November 2019

Ceria-Zirconia/Zeolite Bifunctional Catalyst for Highly Selective Conversion of Syngas into Aromatics journal, August 2018

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Engineering Nanoceria for Enhanced Peroxidase Mimics: A Solid Solution Strategy journal, December 2018

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Title: Mesoporous MnCeO_x solid solutions for low temperature and selective oxidation of hydrocarbons

Green, Catalytic Oxidation of Alcohols in Water
journal, March 2000

Solvent-Free Oxidation of Primary Alcohols to Aldehydes Using Au-Pd/TiO ₂ Catalysts
journal, January 2006

Free Radical Functionalization of Organic Compounds Catalyzed by N- Hydroxyphthalimide ^†
journal, September 2007

Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity
journal, August 2013

Mesoporous Co ₃ O ₄ and Au/Co ₃ O ₄ Catalysts for Low-Temperature Oxidation of Trace Ethylene
journal, March 2010

Efficient stereo- and regioselective hydroxylation of alkanes catalysed by a bulky polyoxometalate
journal, May 2010

Recent Advances in Transition Metal Catalyzed Oxidation of Organic Substrates with Molecular Oxygen
journal, June 2005

CHEMISTRY: Palladium-Catalyzed Oxidation of Organic Chemicals with O2
journal, September 2005

A data-intensive approach to mechanistic elucidation applied to chiral anion catalysis
journal, February 2015

Solvent-Free Oxidation of Primary Carbon-Hydrogen Bonds in Toluene Using Au-Pd Alloy Nanoparticles
journal, January 2011

Overcoming the limitations of directed C–H functionalizations of heterocycles
journal, November 2014

Interfacial Effects in Iron-Nickel Hydroxide-Platinum Nanoparticles Enhance Catalytic Oxidation
journal, May 2014

Tuning Selectivity in Propylene Epoxidation by Plasmon Mediated Photo-Switching of Cu Oxidation State
journal, March 2013

Adding Aliphatic C-H Bond Oxidations to Synthesis
journal, February 2012

Metal-free oxidation of aromatic carbon–hydrogen bonds through a reverse-rebound mechanism
journal, July 2013

Conversion of 1-alkenes into 1,4-diols through an auxiliary-mediated formal homoallylic C–H oxidation
journal, January 2014

Reactivity of the Gold/Water Interface During Selective Oxidation Catalysis
journal, September 2010

CHEMISTRY: Selective Hydrocarbon Oxidation in Zeolites
journal, July 2006

Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst
journal, June 2006

Highly Selective Liquid-Phase Oxidation of Cyclohexane to KA Oil over Ti-MWW Catalyst: Evidence of Formation of Oxyl Radicals
journal, December 2013

Alkane Oxidation with Molecular Oxygen Using a New Efficient Catalytic System: N -Hydroxyphthalimide (NHPI) Combined with Co(acac) _n ( n = 2 or 3) ^†
journal, January 1996

Effective catalysis of simple metalloporphyrins for cyclohexane oxidation with air in the absence of additives and solvents
journal, June 2003

Designing a Heterogeneous Catalyst for the Production of Adipic Acid by Aerial Oxidation of Cyclohexane
journal, July 2000

Aerobic Oxidation of Cyclohexane Catalyzed by Size-Controlled Au Clusters on Hydroxyapatite: Size Effect in the Sub-2 nm Regime
journal, December 2010

Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions
journal, October 2005

Selective oxidation with dioxygen by gold nanoparticle catalysts derived from 55-atom clusters
journal, August 2008

Metal-Free Activation of Dioxygen by Graphene/g-C ₃ N ₄ Nanocomposites: Functional Dyads for Selective Oxidation of Saturated Hydrocarbons
journal, June 2011

Selective Catalysis of the Aerobic Oxidation of Cyclohexane in the Liquid Phase by Carbon Nanotubes
journal, March 2011

Recent Advances in Manganese Oxide Nanocrystals: Fabrication, Characterization, and Microstructure
journal, March 2012

MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures
journal, July 2004

Nanostructured manganese doped ceria solid solutions for CO oxidation at lower temperatures
journal, January 2015

VOC oxidation over MnOx–CeO2 catalysts prepared by a combustion method
journal, October 2008

A theoretic insight into the catalytic activity promotion of CeO2 surfaces by Mn doping
journal, January 2012

Catalytic combustion of chlorobenzene over MnOx–CeO2 mixed oxide catalysts
journal, February 2009

Surfactant-Assisted Synthesis, Characterizations, and Catalytic Oxidation Mechanisms of the Mesoporous MnOx−CeO ₂ and Pd/MnOx−CeO ₂ Catalysts Used for CO and C ₃ H ₈ Oxidation
journal, November 2009

Catalytic removal of benzene over CeO2–MnOx composite oxides prepared by hydrothermal method
journal, July 2013

Structure, Bonding, and Catalytic Activity of Monodisperse, Transition-Metal-Substituted CeO ₂ Nanoparticles
journal, November 2014

“Host−Guest” Chemistry in the Synthesis of Ordered Nonsiliceous Mesoporous Materials
journal, July 2006

Generalized syntheses of large-pore mesoporous metal oxides with semicrystalline frameworks
journal, November 1998

Unique Spatial Heterogeneity in Ionic Liquids
journal, September 2005

A general approach to crystalline and monomodal pore size mesoporous materials
journal, December 2013

Updating Biomass into Functional Carbon Material in Ionothermal Manner
journal, July 2014

The chemical nature of the C–H⊕⋯X− (X=Cl or Br) interaction in imidazolium halide ionic liquids
journal, January 2006

The Structure of a Room-Temperature Ionic Liquid with and without Trace Amounts of Water: The Role of CH⋅⋅⋅O and CH⋅⋅⋅F Interactions in 1-n-Butyl-3-Methylimidazolium Tetrafluoroborate
journal, September 2003

High thermal stability of ceria-based mixed oxide catalysts supported on ZrO2 for toluene combustion
journal, January 2013

Metal organic frameworks (MOFs) as catalysts: A combination of Cu2+ and Co2+ MOFs as an efficient catalyst for tetralin oxidation
journal, April 2008

The Structure of a Room-Temperature Ionic Liquid with and without Trace Amounts of Water: The Role of CH⋅⋅⋅O and CH⋅⋅⋅F Interactions in 1-n-Butyl-3-Methylimidazolium Tetrafluoroborate
journal, September 2003

Recent Advances in Transition Metal Catalyzed Oxidation of Organic Substrates with Molecular Oxygen
journal, October 2005

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journal, December 2007

“Host—Guest” Chemistry in the Synthesis of Ordered Nonsiliceous Mesoporous Materials
journal, October 2006

Selective Catalysis of the Aerobic Oxidation of Cyclohexane in the Liquid Phase by Carbon Nanotubes
journal, March 2011

Free Radical Functionalization of Organic Compounds Catalyzed by N-Hydroxyphthalimide
journal, December 2007

VOC oxidation over MnOx–CeO2 catalysts prepared by a combustion method
journal, October 2008

Updating Biomass into Functional Carbon Material in Ionothermal Manner
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journal, June 2005

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Unique Spatial Heterogeneity in Ionic Liquids
journal, September 2005

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journal, June 2011

Mesoporous Co ₃ O ₄ and Au/Co ₃ O ₄ Catalysts for Low-Temperature Oxidation of Trace Ethylene
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Metal-free oxidation of aromatic carbon–hydrogen bonds through a reverse-rebound mechanism
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Overcoming the limitations of directed C–H functionalizations of heterocycles
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A general approach to crystalline and monomodal pore size mesoporous materials
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Reactivity of the Gold/Water Interface During Selective Oxidation Catalysis
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Selective One‐Step Aerobic Oxidation of Cyclohexane to ϵ‐Caprolactone Mediated by N ‐Hydroxyphthalimide (NHPI)
journal, March 2019

Interfacial CoO _x Layers on TiO ₂ as an Efficient Catalyst for Solvent-Free Aerobic Oxidation of Hydrocarbons
journal, October 2018

Atmospheric Selective Oxidation of Benzyl Alcohol Catalyzed by Pd Nanoparticles Supported on CeO ₂ with Various Morphologies
journal, May 2019

Cooperative Effect of the Ce–Co‐O _x for the Catalytic Oxidation of Toluene
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