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  • American Association for the Advancement of Science (AAAS)  (2)
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  • American Association for the Advancement of Science (AAAS)  (2)
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  • 1
    Online Resource
    Online Resource
    American Association for the Advancement of Science (AAAS) ; 2008
    In:  Science Vol. 322, No. 5898 ( 2008-10-03), p. 73-77
    In: Science, American Association for the Advancement of Science (AAAS), Vol. 322, No. 5898 ( 2008-10-03), p. 73-77
    Abstract: Butenes and butadiene, which are useful intermediates for the synthesis of polymers and other compounds, are synthesized traditionally by oxidative dehydrogenation (ODH) of n -butane over complex metal oxides. Such catalysts require high O 2 /butane ratios to maintain the activity, which leads to unwanted product oxidation. We show that carbon nanotubes with modified surface functionality efficiently catalyze the oxidative dehydrogenation of n -butane to butenes, especially butadiene. For low O 2 /butane ratios, a high selectivity to alkenes was achieved for periods as long as 100 hours. This process is mildly catalyzed by ketonic C O groups and occurs via a combination of parallel and sequential oxidation steps. A small amount of phosphorus greatly improved the selectivity by suppressing the combustion of hydrocarbons.
    Type of Medium: Online Resource
    ISSN: 0036-8075 , 1095-9203
    RVK:
    RVK:
    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 2008
    detail.hit.zdb_id: 128410-1
    detail.hit.zdb_id: 2066996-3
    detail.hit.zdb_id: 2060783-0
    SSG: 11
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  • 2
    Online Resource
    Online Resource
    American Association for the Advancement of Science (AAAS) ; 2020
    In:  Science Advances Vol. 6, No. 26 ( 2020-06-26)
    In: Science Advances, American Association for the Advancement of Science (AAAS), Vol. 6, No. 26 ( 2020-06-26)
    Abstract: Borocarbonitrides (BCNs) have emerged as highly selective catalysts for the oxidative dehydrogenation (ODH) reaction. However, there is a lack of in-depth understanding of the catalytic mechanism over BCN catalysts due to the complexity of the surface oxygen functional groups. Here, BCN nanotubes with multiple active sites are synthesized for oxygen-assisted methanol conversion reaction. The catalyst shows a notable activity improvement for methanol conversion (29%) with excellent selectivity to formaldehyde (54%). Kinetic measurements indicate that carboxylic acid groups on BCN are responsible for the formation of dimethyl ether, while the redox catalysis to formaldehyde occurs on both ketonic carbonyl and boron hydroxyl (B─OH) sites. The ODH reaction pathway on the B─OH site is further revealed by in situ infrared, x-ray absorption spectra, and density functional theory. The present work provides physical-chemical insights into the functional mechanism of BCN catalysts, paving the way for further development of the underexplored nonmetallic catalytic systems.
    Type of Medium: Online Resource
    ISSN: 2375-2548
    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 2020
    detail.hit.zdb_id: 2810933-8
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