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Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM-5-Catalyzed Methane Dehydroaromatization.


ABSTRACT: Non-oxidative methane dehydroaromatization is a promising reaction to directly convert natural gas into aromatic hydrocarbons and hydrogen. Commercialization of this technology is hampered by rapid catalyst deactivation because of coking. A novel approach is presented involving selective oxidation of coke during methane dehydroaromatization at 700?°C. Periodic pulsing of oxygen into the methane feed results in substantially higher cumulative product yield with synthesis gas; a H2 /CO ratio close to two is the main side-product of coke combustion. Using 13 C isotope labeling of methane it is demonstrated that oxygen predominantly reacts with molybdenum carbide species. The resulting molybdenum oxides catalyze coke oxidation. Less than one-fifth of the available oxygen reacts with gaseous methane. Combined with periodic regeneration at 550?°C, this strategy is a significant step forward, towards a process for converting methane into liquid hydrocarbons.

SUBMITTER: Kosinov N 

PROVIDER: S-EPMC5132063 | biostudies-literature | 2016 Nov

REPOSITORIES: biostudies-literature

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Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM-5-Catalyzed Methane Dehydroaromatization.

Kosinov Nikolay N   Coumans Ferdy J A G FJ   Uslamin Evgeny E   Kapteijn Freek F   Hensen Emiel J M EJ  

Angewandte Chemie (International ed. in English) 20161028 48


Non-oxidative methane dehydroaromatization is a promising reaction to directly convert natural gas into aromatic hydrocarbons and hydrogen. Commercialization of this technology is hampered by rapid catalyst deactivation because of coking. A novel approach is presented involving selective oxidation of coke during methane dehydroaromatization at 700 °C. Periodic pulsing of oxygen into the methane feed results in substantially higher cumulative product yield with synthesis gas; a H<sub>2</sub> /CO  ...[more]

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