Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds

Ramasamy, Karthikeyan K.; Gray, Michel; Job, Heather; Smith, Colin; Wang, Yong

doi:10.1016/j.cattod.2015.11.045

Title: Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds

Abstract

Here, a highly versatile ethanol conversion process to selectively generate high value compounds is presented here. By changing the reaction temperature, ethanol can be selectively converted to >C₂ alcohols/oxygenates or phenolic compounds over hydrotalcite derived bi-functional MgO–Al₂O₃ catalyst via complex cascade mechanism. Reaction temperature plays a role in whether aldol condensation or the acetone formation is the path taken in changing the product composition. This article contains the catalytic activity comparison between the mono-functional and physical mixture counterpart to the hydrotalcite derived mixed oxides and the detailed discussion on the reaction mechanisms.

Authors:

Ramasamy, Karthikeyan K. ^[1]; Gray, Michel ^[1]; Job, Heather ^[1]; Smith, Colin ^[1]; Wang, Yong ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)

Publication Date:: Wed Feb 03 00:00:00 EST 2016

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1250889

Alternate Identifier(s):: OSTI ID: 1351656

Report Number(s):: PNNL-SA-115950
Journal ID: ISSN 0920-5861; PII: S0920586116300050

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Catalysis Today

Additional Journal Information:: Journal Volume: 269; Journal Issue: C; Journal ID: ISSN 0920-5861

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ethanol; butanol; hydrotalcite; mixed oxides; guerbet

Citation Formats


                    Ramasamy, Karthikeyan K., Gray, Michel, Job, Heather, Smith, Colin, and Wang, Yong. Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds.  United States: N. p., 2016. 
Web.  doi:10.1016/j.cattod.2015.11.045.

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                    Ramasamy, Karthikeyan K., Gray, Michel, Job, Heather, Smith, Colin, & Wang, Yong. Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds.  United States.  https://doi.org/10.1016/j.cattod.2015.11.045

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                    Ramasamy, Karthikeyan K., Gray, Michel, Job, Heather, Smith, Colin, and Wang, Yong. Wed .  
"Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds".  United States.  https://doi.org/10.1016/j.cattod.2015.11.045.  https://www.osti.gov/servlets/purl/1250889.

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@article{osti_1250889,

  title        = {Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds},

  author       = {Ramasamy, Karthikeyan K. and Gray, Michel and Job, Heather and Smith, Colin and Wang, Yong},

  abstractNote = {Here, a highly versatile ethanol conversion process to selectively generate high value compounds is presented here. By changing the reaction temperature, ethanol can be selectively converted to >C2 alcohols/oxygenates or phenolic compounds over hydrotalcite derived bi-functional MgO–Al2O3 catalyst via complex cascade mechanism. Reaction temperature plays a role in whether aldol condensation or the acetone formation is the path taken in changing the product composition. This article contains the catalytic activity comparison between the mono-functional and physical mixture counterpart to the hydrotalcite derived mixed oxides and the detailed discussion on the reaction mechanisms.},

  doi          = {10.1016/j.cattod.2015.11.045},

  journal      = {Catalysis Today},

  number       = C,

  volume       = 269,

  place        = {United States},

  year         = {Wed Feb 03 00:00:00 EST 2016},

  month        = {Wed Feb 03 00:00:00 EST 2016}

}

Copy to clipboard

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https://doi.org/10.1016/j.cattod.2015.11.045

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Works referencing / citing this record:

Recent advances in selective C-C bond coupling for ethanol upgrading over balanced Lewis acid-base catalysts
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Dai, Jingjing; Zhang, Hongbo
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Catalysis Science & Technology, Vol. 9, Issue 8
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Title: Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds

Abstract

Citation Formats

Heterogeneous catalytic synthesis of ethanol from biomass-derived syngas journal, January 2007

Catalyst activity comparison of alcohols over zeolites journal, January 2013

Heterogeneous Catalysts for the Guerbet Coupling of Alcohols journal, June 2013

Self-coupling of secondary alcohols by Ni/CeO2 catalyst journal, July 2013

Conversion of biomass-derived small oxygenates over HZSM-5 and its deactivation mechanism journal, January 2014

Direct Synthesis of n -Butanol from Ethanol over Nonstoichiometric Hydroxyapatite journal, December 2006

Conversion of ethanol to hydrocarbons on hierarchical HZSM-5 zeolites journal, December 2014

Chemocatalytic Conversion of Ethanol into Butadiene and Other Bulk Chemicals journal, May 2013

A comparison of performance of higher alcohols/diesel fuel blends in a diesel engine journal, July 2012

Phenolic resins—100years of progress and their future journal, February 2013

Efficient hydrotalcite-based catalyst for acetone condensation to α-isophorone—scale up aspects and process development journal, November 1998

The Thermal Decomposition of Mg-Al Hydrotalcites: Effects of Interlayer Anions and Characteristics of the Final Structure journal, December 2002

Transesterification of poultry fat with methanol using Mg–Al hydrotalcite derived catalysts journal, January 2007

Structural and Surface Acid/Base Properties of Hydrotalcite-Derived MgAlO Oxides Calcined at Varying Temperatures journal, May 1998

Vapor-phase methanol and ethanol coupling reactions on CuMgAl mixed metal oxides journal, March 2013

Structure and Surface and Catalytic Properties of Mg-Al Basic Oxides journal, September 1998

Structural Requirements and Reaction Pathways in Condensation Reactions of Alcohols on MgyAlOx Catalysts journal, March 2000

Alkali- and nitrate-free synthesis of highly active Mg–Al hydrotalcite-coated alumina for FAME production journal, January 2014

Oxidant-Free Alcohol Dehydrogenation Using a Reusable Hydrotalcite-Supported Silver Nanoparticle Catalyst journal, January 2008

Mg and Al mixed oxides and the synthesis of n-butanol from ethanol journal, February 2012

Chemicals from ethanol – The dehydrogenative route of the ethyl acetate one-pot synthesis journal, January 2011

One-Pot Asymmetric Nitro-Mannich/Hydroamination Cascades for the Synthesis of Pyrrolidine Derivatives: Combining Organocatalysis and Gold Catalysis journal, December 2013

Bifunctional pathways in catalysis by solid acids and bases journal, November 1997

Self-condensation of propanol over solid-base catalysts journal, November 2004

A low-pressure guerbet reaction over magnesium oxide catalyst journal, January 1990

Condensation of alcohol over solid-base catalyst to form higher alcohols journal, January 1992

Bifunctional Condensation Reactions of Alcohols on Basic Oxides Modified by Copper and Potassium journal, May 1998

Review of catalytic systems and thermodynamics for the Guerbet condensation reaction and challenges for biomass valorization journal, January 2015

Conversion of ethanol to acetone over promoted iron oxide catalysis journal, February 1988

Heterogeneous Basic Catalysis journal, May 1995

Reactions of ethanol over metal oxides journal, March 2000

A study of ZnxZryOz mixed oxides for direct conversion of ethanol to isobutene journal, October 2013

Direct Conversion of Bio-ethanol to Isobutene on Nanosized Zn x Zr y O z Mixed Oxides with Balanced Acid–Base Sites journal, July 2011

Selective catalytic self-condensation of acetone journal, September 1989

Aromatization of isophorone to 3,5-xylenol over Cr2O3/SiO2 catalysts journal, February 2000

Isotopic transient analysis of the ethanol coupling reaction over magnesia journal, February 2013

Recent advances in selective C-C bond coupling for ethanol upgrading over balanced Lewis acid-base catalysts journal, July 2019

Ru Promoted MgO and Al-Modified MgO for Ethanol Upgrading journal, May 2019

Ethanol condensation at elevated pressure over copper on AlMgO and AlCaO porous mixed-oxide supports journal, January 2019

Heterogeneous catalytic synthesis of ethanol from biomass-derived syngas
journal, January 2007

Catalyst activity comparison of alcohols over zeolites
journal, January 2013

Heterogeneous Catalysts for the Guerbet Coupling of Alcohols
journal, June 2013

Self-coupling of secondary alcohols by Ni/CeO2 catalyst
journal, July 2013

Conversion of biomass-derived small oxygenates over HZSM-5 and its deactivation mechanism
journal, January 2014

Direct Synthesis of n -Butanol from Ethanol over Nonstoichiometric Hydroxyapatite
journal, December 2006

Conversion of ethanol to hydrocarbons on hierarchical HZSM-5 zeolites
journal, December 2014

Chemocatalytic Conversion of Ethanol into Butadiene and Other Bulk Chemicals
journal, May 2013

A comparison of performance of higher alcohols/diesel fuel blends in a diesel engine
journal, July 2012

Phenolic resins—100years of progress and their future
journal, February 2013

Efficient hydrotalcite-based catalyst for acetone condensation to α-isophorone—scale up aspects and process development
journal, November 1998

The Thermal Decomposition of Mg-Al Hydrotalcites: Effects of Interlayer Anions and Characteristics of the Final Structure
journal, December 2002

Transesterification of poultry fat with methanol using Mg–Al hydrotalcite derived catalysts
journal, January 2007

Structural and Surface Acid/Base Properties of Hydrotalcite-Derived MgAlO Oxides Calcined at Varying Temperatures
journal, May 1998

Vapor-phase methanol and ethanol coupling reactions on CuMgAl mixed metal oxides
journal, March 2013

Structure and Surface and Catalytic Properties of Mg-Al Basic Oxides
journal, September 1998

Structural Requirements and Reaction Pathways in Condensation Reactions of Alcohols on MgyAlOx Catalysts
journal, March 2000

Alkali- and nitrate-free synthesis of highly active Mg–Al hydrotalcite-coated alumina for FAME production
journal, January 2014

Oxidant-Free Alcohol Dehydrogenation Using a Reusable Hydrotalcite-Supported Silver Nanoparticle Catalyst
journal, January 2008

Mg and Al mixed oxides and the synthesis of n-butanol from ethanol
journal, February 2012

Chemicals from ethanol – The dehydrogenative route of the ethyl acetate one-pot synthesis
journal, January 2011

One-Pot Asymmetric Nitro-Mannich/Hydroamination Cascades for the Synthesis of Pyrrolidine Derivatives: Combining Organocatalysis and Gold Catalysis
journal, December 2013

Bifunctional pathways in catalysis by solid acids and bases
journal, November 1997

Self-condensation of propanol over solid-base catalysts
journal, November 2004

A low-pressure guerbet reaction over magnesium oxide catalyst
journal, January 1990

Condensation of alcohol over solid-base catalyst to form higher alcohols
journal, January 1992

Bifunctional Condensation Reactions of Alcohols on Basic Oxides Modified by Copper and Potassium
journal, May 1998

Review of catalytic systems and thermodynamics for the Guerbet condensation reaction and challenges for biomass valorization
journal, January 2015

Conversion of ethanol to acetone over promoted iron oxide catalysis
journal, February 1988

Heterogeneous Basic Catalysis
journal, May 1995

Reactions of ethanol over metal oxides
journal, March 2000

A study of ZnxZryOz mixed oxides for direct conversion of ethanol to isobutene
journal, October 2013

Direct Conversion of Bio-ethanol to Isobutene on Nanosized Zn _x Zr _y O _z Mixed Oxides with Balanced Acid–Base Sites
journal, July 2011

Selective catalytic self-condensation of acetone
journal, September 1989

Aromatization of isophorone to 3,5-xylenol over Cr2O3/SiO2 catalysts
journal, February 2000

Isotopic transient analysis of the ethanol coupling reaction over magnesia
journal, February 2013

Recent advances in selective C-C bond coupling for ethanol upgrading over balanced Lewis acid-base catalysts
journal, July 2019

Ru Promoted MgO and Al-Modified MgO for Ethanol Upgrading
journal, May 2019

Ethanol condensation at elevated pressure over copper on AlMgO and AlCaO porous mixed-oxide supports
journal, January 2019