Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM-5-Catalyzed Methane Dehydroaromatization.
Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM-5-Catalyzed Methane Dehydroaromatization.
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DOI：
10.1002/anie.201609442
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发表时间：
2016-11-21
影响因子：
16.6
通讯作者：
Hensen, Emiel J. M.
中科院分区：
文献类型：
--
作者：
Kosinov, Nikolay;Coumans, Ferdy J. A. G.;Uslamin, Evgeny;Kapteijn, Freek;Hensen, Emiel J. M.
非氧化甲烷脱氢芳构化是将天然气直接转化为芳烃和氢气的有前途的反应。该技术的商业化受到由于焦化导致的催化剂快速失活的阻碍。提出了一种在700 °C下甲烷脱氢芳构化过程中焦炭选择性氧化的新方法。将氧气周期性地脉冲输送到甲烷进料中导致合成气的累积产物产率显著更高;接近2的H2/CO比是焦炭燃烧的主要副产物。使用13 C同位素标记的甲烷，它表明，氧主要与碳化钼物种反应。所得钼氧化物催化焦炭氧化。只有不到五分之一的氧气会与气态甲烷发生反应。结合550 °C下的定期再生，这一策略是朝着将甲烷转化为液态烃的过程迈出的重要一步。
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 13C 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.
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