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Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM‐5‐Catalyzed Methane Dehydroaromatization
Author(s) -
Kosinov Nikolay,
Coumans Ferdy J. A. G.,
Uslamin Evgeny,
Kapteijn Freek,
Hensen Emiel J. M.
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201609442
Subject(s) - methane , coke , chemistry , catalysis , oxygen , molybdenum , inorganic chemistry , hydrocarbon , hydrogen , combustion , oxygenate , organic chemistry
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 2 /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.