Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane

Love, Alyssa M.; Cendejas, Melissa C.; Thomas, Brijith; McDermott, William P.; Uchupalanun, Pajean; Kruszynski, Catherine; Burt, Samuel P.; Agbi, Theodore; Rossini, Aaron J.; Hermans, Ive

doi:10.1021/acs.jpcc.9b07429

Title: Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane

Abstract

We report on the oxidative dehydrogenation (ODH) activity of silica-supported boron oxide prepared via incipient wetness impregnation. Characterization of pristine and spent catalysts with infrared, Raman, and solid-state NMR spectroscopy reveals the presence of both isolated and aggregated oxidized boron sites. The results of these investigations, in combination with our earlier work on bulk boron-containing ODH catalysts (e.g., h-BN, metal borides, and elemental boron), give direct evidence that oxidized boron species formed in situ on the surface of these materials are responsible for the exceptional catalytic behavior. Furthermore, we anticipate that investigation of supported boron materials can provide insight into the structural characteristics required for selective boron-containing ODH catalysts.

Authors:

Love, Alyssa M. ^[1]; Cendejas, Melissa C. ^[1]; Thomas, Brijith ^[2]; McDermott, William P. ^[1]; Uchupalanun, Pajean ^[1]; Kruszynski, Catherine ^[1]; Burt, Samuel P. ^[1]; Agbi, Theodore ^[1];

^[3];

^[1]

Univ. of Wisconsin, Madison, WI (United States)
Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Publication Date:: Mon Oct 14 00:00:00 EDT 2019

Research Org.:: Ames Lab., Ames, IA (United States); Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1579931

Alternate Identifier(s):: OSTI ID: 1866368

Report Number(s):: IS-J-10107
Journal ID: ISSN 1932-7447

Grant/Contract Number:: SC0017918; AC02-07CH11358; CBET-1605101; CBET-1916809; P41GM66326; P41GM103399

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 123; Journal Issue: 44; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 03 NATURAL GAS; 36 MATERIALS SCIENCE; 42 ENGINEERING; Boron, Boron Nitride, Boron-Based Catalysis, Propane, Propylene, Oxidative Dehydrogenation, Light Alkanes, Olefins, Silica, Solid-State NMR

Citation Formats


                    Love, Alyssa M., Cendejas, Melissa C., Thomas, Brijith, McDermott, William P., Uchupalanun, Pajean, Kruszynski, Catherine, Burt, Samuel P., Agbi, Theodore, Rossini, Aaron J., and Hermans, Ive. Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane.  United States: N. p., 2019. 
Web.  doi:10.1021/acs.jpcc.9b07429.

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                    Love, Alyssa M., Cendejas, Melissa C., Thomas, Brijith, McDermott, William P., Uchupalanun, Pajean, Kruszynski, Catherine, Burt, Samuel P., Agbi, Theodore, Rossini, Aaron J., & Hermans, Ive. Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane.  United States.  https://doi.org/10.1021/acs.jpcc.9b07429

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                    Love, Alyssa M., Cendejas, Melissa C., Thomas, Brijith, McDermott, William P., Uchupalanun, Pajean, Kruszynski, Catherine, Burt, Samuel P., Agbi, Theodore, Rossini, Aaron J., and Hermans, Ive. Mon .  
"Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane".  United States.  https://doi.org/10.1021/acs.jpcc.9b07429.  https://www.osti.gov/servlets/purl/1579931.

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@article{osti_1579931,

  title        = {Synthesis and Characterization of Silica-Supported Boron Oxide Catalysts for the Oxidative Dehydrogenation of Propane},

  author       = {Love, Alyssa M. and Cendejas, Melissa C. and Thomas, Brijith and McDermott, William P. and Uchupalanun, Pajean and Kruszynski, Catherine and Burt, Samuel P. and Agbi, Theodore and Rossini, Aaron J. and Hermans, Ive},

  abstractNote = {We report on the oxidative dehydrogenation (ODH) activity of silica-supported boron oxide prepared via incipient wetness impregnation. Characterization of pristine and spent catalysts with infrared, Raman, and solid-state NMR spectroscopy reveals the presence of both isolated and aggregated oxidized boron sites. The results of these investigations, in combination with our earlier work on bulk boron-containing ODH catalysts (e.g., h-BN, metal borides, and elemental boron), give direct evidence that oxidized boron species formed in situ on the surface of these materials are responsible for the exceptional catalytic behavior. Furthermore, we anticipate that investigation of supported boron materials can provide insight into the structural characteristics required for selective boron-containing ODH catalysts.},

  doi          = {10.1021/acs.jpcc.9b07429},

  journal      = {Journal of Physical Chemistry. C},

  number       = 44,

  volume       = 123,

  place        = {United States},

  year         = {Mon Oct 14 00:00:00 EDT 2019},

  month        = {Mon Oct 14 00:00:00 EDT 2019}

}

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https://doi.org/10.1021/acs.jpcc.9b07429

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Cited by: 40 works

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Figures / Tables:

Figure 1: a) Propylene selectivity versus propane conversion data for the oxidative dehydrogenation (ODH) of propane over a series of B/SiO₂ catalysts (0.23, 0.46, 0.58, 1.2, and 1.7 wt. % B) and h-BN. Different conversions were achieved by changing the gas flow rate between 40 and 200 mL min^-1. b)more »

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