Enhanced Methane Conversion to Olefins and Aromatics by H-Donor Molecules under Nonoxidative Condition
Enhanced Methane Conversion to Olefins and Aromatics by H-Donor Molecules under Nonoxidative Condition
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DOI：
10.1021/acscatal.9b01771
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发表时间：
2019-10-01
期刊：
影响因子：
12.9
通讯作者：
Bao, Xinhe
中科院分区：
文献类型：
--
作者：
Hao, Jianqi;Schwach, Pierre;Bao, Xinhe
我们报道了在铁涂层催化石英反应器上甲烷转化为烯烃和芳烃的反应可以被氢自由基的促进，氢自由基是由氢供体分子如1，2，3，4-四氢萘(THN)和苯的热分解提供的。在1323K下，当甲烷中THN含量为1.41%时，甲烷转化率从19.7%提高到25.5%；在甲烷原料中加入7.7%的C6H6，C2H4生成的起始温度从1143 K降低到1073 K。同位素实验进一步表明，H自由基参与了该反应，根据该反应可以均匀地活化甲烷：中心点H+CH4->；H-2+中心点CH3；这是除了甲烷在铁位上的多相活化之外发生的。
We report that methane conversion to olefins and aromatics over an iron-coated catalytic quartz reactor can be enhanced by hydrogen radicals, which are provided by the thermal decomposition of hydrogen-donor molecules, such as 1,2,3,4-tetrahydronaphthalene (THN) and benzene. For example, methane conversion increases from 19.7% to 25.5% in the presence of 1.41% THN in methane at 1323 K. The onset temperature of C2H4 formation decreases from 1143 to 1073 K by adding 7.7% C6H6 into the methane feed. Isotope experiments further indicate the involvement of H radicals in the reaction, which could activate methane homogeneously according to the reaction: center dot H + CH4 -> H-2 + center dot CH3; this occurs in addition to the heterogeneous activation of methane over iron sites.