Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C3–C5 Olefins over ZnxZryOz Catalyst

doi:10.3390/catal9110923

Title: Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C ₃–C ₅ Olefins over Zn _xZr _yO _z Catalyst

Abstract

The viability of using a Zn _xZr _yO _z mixed oxide catalyst for the direct production of C ₄ olefins from the aqueous phase derived from three different bio-oils was explored. The aqueous phases derived from (i) hydrothermal liquefaction of corn stover, (ii) fluidized bed fast pyrolysis of horse litter, and (iii) screw pyrolysis of wood pellets were evaluated as feedstocks. While exact compositions vary, the primary constituents for each feedstock are acetic acid and propionic acid. Continuous processing, based on liquid–liquid extraction, for the cleanup of the inorganic contaminants contained in the aqueous phase was also demonstrated. Complete conversion of the carboxylic acids was achieved over Zn _xZr _yO _z catalyst for all the feedstocks investigated. The main reaction products from each of the feedstocks include isobutene (>30% selectivity) and CO ₂ (>23% selectivity). Activity loss from coking was also observed, thereby rendering deactivation of the Zn _xZr _yO _z catalyst, however, complete recovery of catalyst activity was observed following regeneration. Finally, the presence of H ₂ in the feed was found to facilitate hydrogenation of intermediate acetone, thereby increasing propene production and, consequently, decreasing isobutene production.

Authors:

^[1];

^[1]; Flake, Matthew D. ^[1]; Cooper, Alan R. ^[1]; Elkasabi, Yaseen ^[2];

^[3]; Lebarbier Dagle, Vanessa ^[1]; Albrecht, Karl O. ^[4];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate, Inst. for Integrated Catalysis
USDA-ARS Eastern Regional Research Center, Wyndmoor, PA (United States)
ARCUS Greencycling Technologies GmbH, Ludwigsburg (Germany)
Archer Daniels Midland Co., Decatur, IL (United States). James R. Randall Research Center

Publication Date:: 2019-11-06

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1574663

Report Number(s):: PNNL-SA-148421
Journal ID: ISSN 2073-4344; CATACJ

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Catalysts

Additional Journal Information:: Journal Volume: 9; Journal Issue: 11; Journal ID: ISSN 2073-4344

Publisher:: MDPI

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; biomass-derived aqueous phase upgrading; olefin production; oxide catalyst

Citation Formats


                    Davidson, Stephen D., Lopez-Ruiz, Juan A., Flake, Matthew D., Cooper, Alan R., Elkasabi, Yaseen, Tomasi Morgano, Marco, Lebarbier Dagle, Vanessa, Albrecht, Karl O., and Dagle, Robert A. Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C3–C5 Olefins over ZnxZryOz Catalyst.  United States: N. p., 2019. 
        Web.  doi:10.3390/catal9110923.

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                    Davidson, Stephen D., Lopez-Ruiz, Juan A., Flake, Matthew D., Cooper, Alan R., Elkasabi, Yaseen, Tomasi Morgano, Marco, Lebarbier Dagle, Vanessa, Albrecht, Karl O., & Dagle, Robert A. Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C3–C5 Olefins over ZnxZryOz Catalyst.  United States.  doi:10.3390/catal9110923.

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                    Davidson, Stephen D., Lopez-Ruiz, Juan A., Flake, Matthew D., Cooper, Alan R., Elkasabi, Yaseen, Tomasi Morgano, Marco, Lebarbier Dagle, Vanessa, Albrecht, Karl O., and Dagle, Robert A. Wed .  
        "Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C3–C5 Olefins over ZnxZryOz Catalyst".  United States.  doi:10.3390/catal9110923.  https://www.osti.gov/servlets/purl/1574663.

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@article{osti_1574663,

  title        = {Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C3–C5 Olefins over ZnxZryOz Catalyst},

  author       = {Davidson, Stephen D. and Lopez-Ruiz, Juan A. and Flake, Matthew D. and Cooper, Alan R. and Elkasabi, Yaseen and Tomasi Morgano, Marco and Lebarbier Dagle, Vanessa and Albrecht, Karl O. and Dagle, Robert A.},

  abstractNote = {The viability of using a ZnxZryOz mixed oxide catalyst for the direct production of C4 olefins from the aqueous phase derived from three different bio-oils was explored. The aqueous phases derived from (i) hydrothermal liquefaction of corn stover, (ii) fluidized bed fast pyrolysis of horse litter, and (iii) screw pyrolysis of wood pellets were evaluated as feedstocks. While exact compositions vary, the primary constituents for each feedstock are acetic acid and propionic acid. Continuous processing, based on liquid–liquid extraction, for the cleanup of the inorganic contaminants contained in the aqueous phase was also demonstrated. Complete conversion of the carboxylic acids was achieved over ZnxZryOz catalyst for all the feedstocks investigated. The main reaction products from each of the feedstocks include isobutene (>30% selectivity) and CO2 (>23% selectivity). Activity loss from coking was also observed, thereby rendering deactivation of the ZnxZryOz catalyst, however, complete recovery of catalyst activity was observed following regeneration. Finally, the presence of H2 in the feed was found to facilitate hydrogenation of intermediate acetone, thereby increasing propene production and, consequently, decreasing isobutene production.},

  doi          = {10.3390/catal9110923},

  journal      = {Catalysts},

  number       = 11,

  volume       = 9,

  place        = {United States},

  year         = {2019},

  month        = {11}

}

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DOI: 10.3390/catal9110923

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Title: Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C 3–C 5 Olefins over Zn xZr yO z Catalyst

Abstract

Citation Formats

Synthesis of Transportation Fuels from Biomass: Chemistry, Catalysts, and Engineering journal, September 2006

Production of renewable jet fuel range alkanes and commodity chemicals from integrated catalytic processing of biomass journal, January 2014

Synergies between Bio- and Oil Refineries for the Production of Fuels from Biomass journal, September 2007

Techno-economic analysis of liquid fuel production from woody biomass via hydrothermal liquefaction (HTL) and upgrading journal, September 2014

Liquid-Phase Catalytic Processing of Biomass-Derived Oxygenated Hydrocarbons to Fuels and Chemicals journal, September 2007

Characterization of the aqueous fractions from hydrotreatment and hydrothermal liquefaction of lignocellulosic feedstocks journal, March 2015

Review of biomass pyrolysis oil properties and upgrading research journal, January 2007

Developments in direct thermochemical liquefaction of biomass: 1983-1990 journal, May 1991

Hydrothermal liquefaction of biomass: Developments from batch to continuous process journal, February 2015

Experimental comparison of two bench scale units for fast and intermediate pyrolysis journal, March 2017

Bench-Scale Fluidized-Bed Pyrolysis of Switchgrass for Bio-Oil Production † journal, March 2007

An overview of aqueous-phase catalytic processes for production of hydrogen and alkanes in a biorefinery journal, January 2006

Oligomerization of ethanol-derived propene and isobutene mixtures to transportation fuels: catalyst and process considerations journal, January 2019

Integrated process for the catalytic conversion of biomass-derived syngas into transportation fuels journal, January 2016

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

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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

Conversion of syngas-derived C2+ mixed oxygenates to C3–C5 olefins over ZnxZryOz mixed oxide catalysts journal, January 2016

Single‐step Conversion of Methyl Ethyl Ketone to Olefins over Zn x Zr y O z Catalysts in Water journal, June 2019

Cascade Reactions for the Continuous and Selective Production of Isobutene from Bioderived Acetic Acid Over Zinc-Zirconia Catalysts journal, October 2014

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Title: Cleanup and Conversion of Biomass Liquefaction Aqueous Phase to C ₃–C ₅ Olefins over Zn _xZr _yO _z Catalyst

Synthesis of Transportation Fuels from Biomass: Chemistry, Catalysts, and Engineering
journal, September 2006

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journal, January 2014

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journal, September 2007

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Liquid-Phase Catalytic Processing of Biomass-Derived Oxygenated Hydrocarbons to Fuels and Chemicals
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journal, February 2015

Experimental comparison of two bench scale units for fast and intermediate pyrolysis
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Bench-Scale Fluidized-Bed Pyrolysis of Switchgrass for Bio-Oil Production ^†
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journal, April 1998

A study of ZnxZryOz mixed oxides for direct conversion of ethanol to isobutene
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Key Roles of Lewis Acid–Base Pairs on Zn _x Zr _y O _z in Direct Ethanol/Acetone to Isobutene Conversion
journal, December 2015

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

Conversion of syngas-derived C₂+ mixed oxygenates to C₃–C₅ olefins over Zn_xZr_yO_z mixed oxide catalysts
journal, January 2016

Single‐step Conversion of Methyl Ethyl Ketone to Olefins over Zn _x Zr _y O _z Catalysts in Water
journal, June 2019

Cascade Reactions for the Continuous and Selective Production of Isobutene from Bioderived Acetic Acid Over Zinc-Zirconia Catalysts
journal, October 2014

Production of Deoxygenated Biomass Fast Pyrolysis Oils via Product Gas Recycling
journal, June 2013

Mobile demonstration unit for fast- and catalytic pyrolysis: The combustion reduction integrated pyrolysis system (CRIPS)
journal, January 2019

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journal, May 2015

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