Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5

doi:10.1039/C7GC01188A

Title: Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5

Abstract

Selective conversion of bio-derived ethanol to benzene, toluene and xylenes (BTX) is desirable for producing renewable BTX. Here in this work, we show that addition of Ga to H-ZSM-5 leads to two-fold increase in the BTX yield as compared with H-ZSM-5 when ethanol is converted over these zeolites at 450 °C and ambient pressure. Besides promoting BTX formation, Ga also plays an important role in enhancing molecular hydrogen production and suppressing hydrogen transfer reactions for light alkane formation. The ion exchange synthesis of Ga-ZSM-5 results in the majority of Ga at the outer surface of zeolite crystals as extra-zeolitic Ga ₂O ₃ particles and only a small fraction of Ga exchanging with the Brønsted acid sites which appears to be responsible for higher ethanol conversion to BTX. The interface between H-ZSM-5 and Ga ₂O ₃ particles is not active since H-ZSM-5 and physical mixture of β-Ga ₂O ₃/H-ZSM-5 furnish almost identical product distribution. Hydrogen reduction of the physical mixtures facilitates movement of Ga to ion exchange locations and dramatically increases BTX yield becoming comparable to those obtained over ion-exchanged Ga-ZSM-5, suggesting that exchanged Ga(III) cations are responsible for the increased BTX production. Linear correlation between BTX site time yield andmore »« less

Authors:

^[1]; Lepore, Andrew W. ^[2]; Salazar, Mariam F. ^[3];

^[4];

^[5];

^[6];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy & Transportation Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioSciences Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

Publication Date:: 2017-06-01

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

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI Identifier:: 1394295

DOE Contract Number:: AC05-00OR22725

Resource Type:: Journal Article

Journal Name:: Green Chemistry

Additional Journal Information:: Journal Volume: 19; Journal Issue: 18; Journal ID: ISSN 1463-9262

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 09 BIOMASS FUELS

Citation Formats


                    Li, Zhenglong, Lepore, Andrew W., Salazar, Mariam F., Foo, Guo Shiou, Davison, Brian H., Wu, Zili, and Narula, Chaitanya Kumar. Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5.  United States: N. p., 2017. 
        Web.  doi:10.1039/C7GC01188A.

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                    Li, Zhenglong, Lepore, Andrew W., Salazar, Mariam F., Foo, Guo Shiou, Davison, Brian H., Wu, Zili, & Narula, Chaitanya Kumar. Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5.  United States.  doi:10.1039/C7GC01188A.

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                    Li, Zhenglong, Lepore, Andrew W., Salazar, Mariam F., Foo, Guo Shiou, Davison, Brian H., Wu, Zili, and Narula, Chaitanya Kumar. Thu .  
        "Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5".  United States.  doi:10.1039/C7GC01188A.

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@article{osti_1394295,

  title        = {Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5},

  author       = {Li, Zhenglong and Lepore, Andrew W. and Salazar, Mariam F. and Foo, Guo Shiou and Davison, Brian H. and Wu, Zili and Narula, Chaitanya Kumar},

  abstractNote = {Selective conversion of bio-derived ethanol to benzene, toluene and xylenes (BTX) is desirable for producing renewable BTX. Here in this work, we show that addition of Ga to H-ZSM-5 leads to two-fold increase in the BTX yield as compared with H-ZSM-5 when ethanol is converted over these zeolites at 450 °C and ambient pressure. Besides promoting BTX formation, Ga also plays an important role in enhancing molecular hydrogen production and suppressing hydrogen transfer reactions for light alkane formation. The ion exchange synthesis of Ga-ZSM-5 results in the majority of Ga at the outer surface of zeolite crystals as extra-zeolitic Ga2O3 particles and only a small fraction of Ga exchanging with the Brønsted acid sites which appears to be responsible for higher ethanol conversion to BTX. The interface between H-ZSM-5 and Ga2O3 particles is not active since H-ZSM-5 and physical mixture of β-Ga2O3/H-ZSM-5 furnish almost identical product distribution. Hydrogen reduction of the physical mixtures facilitates movement of Ga to ion exchange locations and dramatically increases BTX yield becoming comparable to those obtained over ion-exchanged Ga-ZSM-5, suggesting that exchanged Ga(III) cations are responsible for the increased BTX production. Linear correlation between BTX site time yield and exchanged Ga sites further confirms that Ga occupying cationic sites are active sites for enhancing BTX formation. Reduction of physical mixtures (β-Ga2O3/H-ZSM-5) also provides an economical and environmentally friendly non-aqueous method for large scale catalyst synthesis without sacrificing catalyst performance for ethanol conversion application.},

  doi          = {10.1039/C7GC01188A},

  journal      = {Green Chemistry},

  issn         = {1463-9262},

  number       = 18,

  volume       = 19,

  place        = {United States},

  year         = {2017},

  month        = {6}

}

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DOI: 10.1039/C7GC01188A

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Similar Records

Title: Selective Conversion of Bio-Derived Ethanol to Renewable BTX over Ga-ZSM-5

Abstract

Citation Formats

Transformation of butanes over ZSM-5 zeolites. Part 2.—Formation of aromatic hydrocarbons over Zn-ZSM-5 and Ga-ZSM-5 journal, January 1991

Aromatization of dilute ethylene over Ga-modified ZSM-5 type zeolite catalysts journal, October 2001

Recent Advances in Catalytic Conversion of Ethanol to Chemicals journal, March 2014

Technological trends, global market, and challenges of bio-ethanol production journal, November 2010

The Hydrocarbon Pool in Ethanol-to-Gasoline over HZSM-5 Catalysts journal, November 2008

Catalytic dehydration of bioethanol to ethylene over TiO2/γ-Al2O3 catalysts in microchannel reactors journal, July 2007

Structure and function of metal cations in light alkane reactions catalyzed by modified H-ZSM5 journal, December 1996

One-step catalytic conversion of ethanol into 1,3-butadiene using zinc-containing talc journal, August 2015

Microkinetic modeling of propane aromatization over HZSM-5 journal, October 2005

1-Butanol synthesis from ethanol over strontium phosphate hydroxyapatite catalysts with various Sr/P ratios journal, December 2012

Influence of Zn- and Ga-doping on the conversion of ethanol to hydrocarbons over ZSM-5 journal, January 1992

Ga2O3/HZSM-5 propane aromatization catalysts: Formation of active centers via solid-state reaction journal, November 1990

Catalyst Deactivation by Coke in the Transformation of Aqueous Ethanol into Hydrocarbons. Kinetic Modeling and Acidity Deterioration of the Catalyst journal, August 2002

Selective synthesis of 1-butanol from ethanol over strontium phosphate hydroxyapatite catalysts journal, July 2011

Nonoxidative Activation of Methane journal, January 2003

A descriptor for the relative propagation of the aromatic- and olefin-based cycles in methanol-to-hydrocarbons conversion on H-ZSM-5 journal, July 2013

Reaction of ethanol over hydroxyapatite affected by Ca/P ratio of catalyst journal, October 2008

On reaction pathways in the conversion of methanol to hydrocarbons on HZSM-5 journal, August 2014

Catalytic study of the conversion of ethanol into 1,3-butadiene journal, December 2012

Heterobimetallic Zeolite, InV-ZSM-5, Enables Efficient Conversion of Biomass Derived Ethanol to Renewable Hydrocarbons journal, November 2015

Decomposition and Aromatization of Ethanol on ZSM-Based Catalysts journal, November 2006

Catalytic transformation of ethanol into 1,3-butadiene journal, September 2014

Catalytic Conversion of Propane to Aromatics: Effects of Adding Ga and/or Pt to HZSM-5 journal, October 1994

Structure of Mo 2 C x and Mo 4 C x Molybdenum Carbide Nanoparticles and Their Anchoring Sites on ZSM-5 Zeolites journal, February 2014

Reprint of “Ethanol to higher hydrocarbons over Ni, Ga, Fe-modified ZSM-5: Effect of metal content” journal, September 2015

Ethanol transformation into hydrocarbons on ZSM-5 zeolites: Influence of Si/Al ratio on catalytic performances and deactivation rate. Study of the radical species role journal, November 2012

Aromatization of ethanol on Mo2C/ZSM catalysts journal, August 2006

Aromatization of propene and n-butene over H-galloaluminosilicate (ZSM-5 type) zeolite journal, May 2002

Organometallic model complexes elucidate the active gallium species in alkane dehydrogenation catalysts based on ligand effects in Ga K-edge XANES journal, January 2016

Recent trends in global production and utilization of bio-ethanol fuel journal, November 2009

Cracking of n-heptane over Brønsted acid sites and Lewis acid Ga sites in ZSM-5 zeolite journal, April 2008

Catalytic dehydration of bioethanol to ethylene: Pilot-scale studies and process simulation journal, December 2011

Effect of H2–O2 pre-treatments on the state of gallium in Ga/H-ZSM-5 propane aromatisation catalysts journal, September 2003

Transformation of butanes over ZSM-5 zeolites. Part 2.—Formation of aromatic hydrocarbons over Zn-ZSM-5 and Ga-ZSM-5
journal, January 1991

Aromatization of dilute ethylene over Ga-modified ZSM-5 type zeolite catalysts
journal, October 2001

Recent Advances in Catalytic Conversion of Ethanol to Chemicals
journal, March 2014

Technological trends, global market, and challenges of bio-ethanol production
journal, November 2010

The Hydrocarbon Pool in Ethanol-to-Gasoline over HZSM-5 Catalysts
journal, November 2008

Catalytic dehydration of bioethanol to ethylene over TiO2/γ-Al2O3 catalysts in microchannel reactors
journal, July 2007

Structure and function of metal cations in light alkane reactions catalyzed by modified H-ZSM5
journal, December 1996

One-step catalytic conversion of ethanol into 1,3-butadiene using zinc-containing talc
journal, August 2015

Microkinetic modeling of propane aromatization over HZSM-5
journal, October 2005

1-Butanol synthesis from ethanol over strontium phosphate hydroxyapatite catalysts with various Sr/P ratios
journal, December 2012

Influence of Zn- and Ga-doping on the conversion of ethanol to hydrocarbons over ZSM-5
journal, January 1992

Ga2O3/HZSM-5 propane aromatization catalysts: Formation of active centers via solid-state reaction
journal, November 1990

Catalyst Deactivation by Coke in the Transformation of Aqueous Ethanol into Hydrocarbons. Kinetic Modeling and Acidity Deterioration of the Catalyst
journal, August 2002

Selective synthesis of 1-butanol from ethanol over strontium phosphate hydroxyapatite catalysts
journal, July 2011

Nonoxidative Activation of Methane
journal, January 2003

A descriptor for the relative propagation of the aromatic- and olefin-based cycles in methanol-to-hydrocarbons conversion on H-ZSM-5
journal, July 2013

Reaction of ethanol over hydroxyapatite affected by Ca/P ratio of catalyst
journal, October 2008

On reaction pathways in the conversion of methanol to hydrocarbons on HZSM-5
journal, August 2014

Catalytic study of the conversion of ethanol into 1,3-butadiene
journal, December 2012

Heterobimetallic Zeolite, InV-ZSM-5, Enables Efficient Conversion of Biomass Derived Ethanol to Renewable Hydrocarbons
journal, November 2015

Decomposition and Aromatization of Ethanol on ZSM-Based Catalysts
journal, November 2006

Catalytic transformation of ethanol into 1,3-butadiene
journal, September 2014

Catalytic Conversion of Propane to Aromatics: Effects of Adding Ga and/or Pt to HZSM-5
journal, October 1994

Structure of Mo ₂ C _x and Mo ₄ C _x Molybdenum Carbide Nanoparticles and Their Anchoring Sites on ZSM-5 Zeolites
journal, February 2014

Reprint of “Ethanol to higher hydrocarbons over Ni, Ga, Fe-modified ZSM-5: Effect of metal content”
journal, September 2015

Ethanol transformation into hydrocarbons on ZSM-5 zeolites: Influence of Si/Al ratio on catalytic performances and deactivation rate. Study of the radical species role
journal, November 2012

Aromatization of ethanol on Mo2C/ZSM catalysts
journal, August 2006

Aromatization of propene and n-butene over H-galloaluminosilicate (ZSM-5 type) zeolite
journal, May 2002

Organometallic model complexes elucidate the active gallium species in alkane dehydrogenation catalysts based on ligand effects in Ga K-edge XANES
journal, January 2016

Recent trends in global production and utilization of bio-ethanol fuel
journal, November 2009

Cracking of n-heptane over Brønsted acid sites and Lewis acid Ga sites in ZSM-5 zeolite
journal, April 2008

Catalytic dehydration of bioethanol to ethylene: Pilot-scale studies and process simulation
journal, December 2011

Effect of H2–O2 pre-treatments on the state of gallium in Ga/H-ZSM-5 propane aromatisation catalysts
journal, September 2003