Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

Love, Alyssa M.; Thomas, Brijith; Specht, Sarah E.; Hanrahan, Michael P.; Venegas, Juan M.; Burt, Samuel P.; Grant, Joseph T.; Cendejas, Melissa C.; McDermott, William P.; Rossini, Aaron J.; Hermans, Ive

doi:10.1021/jacs.8b08165

Title: Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

Journal Article · Fri Dec 07 00:00:00 UTC 2018 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.8b08165 · OSTI ID:1492337

Love, Alyssa M. ^[1]; Thomas, Brijith ^[2]; Specht, Sarah E. ^[1]; Hanrahan, Michael P. ^[3];

^[1]; Burt, Samuel P. ^[1]; Grant, Joseph T. ^[1]; Cendejas, Melissa C. ^[1]; McDermott, William P. ^[1];

^[3];

^[1]

Univ. of Wisconsin, Madison, WI (United States)
US DOE Ames Laboratory, Ames, Iowa 50011, United States
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Hexagonal boron nitride (h-BN) and boron nitride nanotubes (BNNTs) were recently reported as highly selective catalysts for the oxidative dehydrogenation (ODH) of alkanes to olefins in the gas phase. Previous studies revealed a substantial increase in surface oxygen content after exposure to ODH conditions (heating to ca. 500 °C under a flow of alkane and oxygen); however, the complexity of these materials has thus far precluded an in-depth understanding of the oxygenated surface species. In this contribution, we combine advanced NMR spectroscopy experiments with scanning electron microscopy (SEM) and soft X-ray absorption spectroscopy (XAS) to characterize the molecular structure of the oxygen functionalized phase that arises on h-BN and BNNTs following catalytic testing for ODH of propane. The pristine BN materials are readily oxidized and hydrolyzed under ODH reaction conditions to yield a phase consisting of three coordinate boron sites with variable numbers of hydroxyl and bridging oxide groups which is denoted B(OH)_xO_3-x (where x = 0-3). Evidence for this robust oxide phase revises previous literature hypotheses of hydroxylated BN edges as the active component on h-BN.

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358; SC0017918

OSTI ID:: 1492337

Report Number(s):: IS-J--9850

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 1 Vol. 141; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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03 NATURAL GAS
36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
Boron
Boron nitride
Boron-based catalysis
Light alkanes
Materials
Nitrides
Nuclear magnetic resonance spectroscopy
Olefins
Oxidative dehydrogenation
Propane
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Title: Probing the Transformation of Boron Nitride Catalysts under Oxidative Dehydrogenation Conditions

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References (42)

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