Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation

Baddour, Frederick G.; Witte, Vanessa A.; Nash, Connor P.; Griffin, Michael B.; Ruddy, Daniel A.; Schaidle, Joshua A.

doi:10.1021/acssuschemeng.7b02544

Title: Late-Transition-Metal-Modified β-Mo₂C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation

Abstract

Molybdenum carbide has been identified as a promising bifunctional catalyst in the deoxygenation of a variety of pyrolysis vapor model compounds. Although high deoxygenation activity has been demonstrated, complementary hydrogenation activity has been limited, especially for lignin-derived, aromatic model compounds. The ability to control the relative site densities of acidic and hydrogenation functionalities represents a catalyst design challenge for these materials with the goal to improve hydrogenation activity under ex situ catalytic fast pyrolysis (CFP) conditions. Here in this paper, we demonstrate that the addition of Pt and Ni to Mo₂C resulted in an increase in the H*-site density with only a minor decrease in the acid-site density. In contrast, the addition of Pd did not significantly alter the H* or acid site densities. High conversions (>94%) and high selectivities to 0-oxygen products (>80%) were observed in guaiacol deoxygenation under ex situ CFP conditions (350 °C and 0.44 MPa H₂) for all catalysts. Pt addition resulted in the greatest deoxygenation, and site-time yields to hydrogenated products over the Pt/Mo₂C catalyst were increased to 0.048 s^-1 compared to 0.015-0.019 s^-1 for all other catalysts. The Pt/Mo₂C catalyst demonstrated the highest hydrogenation performance, but modification with Ni also significantly enhanced hydrogenation performance,more »« less

Authors:

Baddour, Frederick G. ^[1]; Witte, Vanessa A. ^[1]; Nash, Connor P. ^[1]; Griffin, Michael B. ^[1];

^[1]; Schaidle, Joshua A. ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States). National Bioenergy Center

Publication Date:: Thu Oct 26 00:00:00 EDT 2017

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office

OSTI Identifier:: 1408685

Report Number(s):: NREL/JA-5100-68710
Journal ID: ISSN 2168-0485

Grant/Contract Number:: AC36-08GO28308

Resource Type:: Accepted Manuscript

Journal Name:: ACS Sustainable Chemistry & Engineering

Additional Journal Information:: Journal Volume: 5; Journal Issue: 12; Journal ID: ISSN 2168-0485

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 09 BIOMASS FUELS; catalytic fast pyrolysis; vapor phase upgrading; deoxygenation; hydrogenation; molybdenum carbide; guaiacol

Citation Formats


                    Baddour, Frederick G., Witte, Vanessa A., Nash, Connor P., Griffin, Michael B., Ruddy, Daniel A., and Schaidle, Joshua A. Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation.  United States: N. p., 2017. 
Web.  doi:10.1021/acssuschemeng.7b02544.

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                    Baddour, Frederick G., Witte, Vanessa A., Nash, Connor P., Griffin, Michael B., Ruddy, Daniel A., & Schaidle, Joshua A. Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation.  United States.  https://doi.org/10.1021/acssuschemeng.7b02544

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                    Baddour, Frederick G., Witte, Vanessa A., Nash, Connor P., Griffin, Michael B., Ruddy, Daniel A., and Schaidle, Joshua A. Thu .  
"Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation".  United States.  https://doi.org/10.1021/acssuschemeng.7b02544.  https://www.osti.gov/servlets/purl/1408685.

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@article{osti_1408685,

  title        = {Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation},

  author       = {Baddour, Frederick G. and Witte, Vanessa A. and Nash, Connor P. and Griffin, Michael B. and Ruddy, Daniel A. and Schaidle, Joshua A.},

  abstractNote = {Molybdenum carbide has been identified as a promising bifunctional catalyst in the deoxygenation of a variety of pyrolysis vapor model compounds. Although high deoxygenation activity has been demonstrated, complementary hydrogenation activity has been limited, especially for lignin-derived, aromatic model compounds. The ability to control the relative site densities of acidic and hydrogenation functionalities represents a catalyst design challenge for these materials with the goal to improve hydrogenation activity under ex situ catalytic fast pyrolysis (CFP) conditions. Here in this paper, we demonstrate that the addition of Pt and Ni to Mo2C resulted in an increase in the H*-site density with only a minor decrease in the acid-site density. In contrast, the addition of Pd did not significantly alter the H* or acid site densities. High conversions (>94%) and high selectivities to 0-oxygen products (>80%) were observed in guaiacol deoxygenation under ex situ CFP conditions (350 °C and 0.44 MPa H2) for all catalysts. Pt addition resulted in the greatest deoxygenation, and site-time yields to hydrogenated products over the Pt/Mo2C catalyst were increased to 0.048 s-1 compared to 0.015-0.019 s-1 for all other catalysts. The Pt/Mo2C catalyst demonstrated the highest hydrogenation performance, but modification with Ni also significantly enhanced hydrogenation performance, representing a promising lower-cost alternative.},

  doi          = {10.1021/acssuschemeng.7b02544},

  journal      = {ACS Sustainable Chemistry & Engineering},

  number       = 12,

  volume       = 5,

  place        = {United States},

  year         = {Thu Oct 26 00:00:00 EDT 2017},

  month        = {Thu Oct 26 00:00:00 EDT 2017}

}

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Title: Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation

Abstract

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