Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 1, Pages 182-190Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b08165
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Funding
- National Science Foundation [CBET-1605101]
- U.S. Department of Energy [DE-SC0017918]
- U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Science and Engineering Division
- U.S. DOE [DE-AC02-07CH11358]
- DOE Office of Science User Facility [DE-AC02-05CH11231]
- U.S. Department of Energy (DOE) [DE-SC0017918] Funding Source: U.S. Department of Energy (DOE)
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Hexagonal boron nitride (h-BN) and boron nitride nanotubes (BNNT) 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 degrees 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 and soft X-ray absorption spectroscopy to characterize the molecular structure of the oxygen functionalized phase that arises on h-BN and BNNT 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)(x)O3-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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