Natural Gas to Fuels and Chemicals: Improved Methane Aromatization in an Oxygen-Permeable Membrane Reactor
Natural Gas to Fuels and Chemicals: Improved Methane Aromatization in an Oxygen-Permeable Membrane Reactor
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DOI：
10.1002/anie.201307935
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发表时间：
2013-12-16
影响因子：
16.6
通讯作者：
Caro, Juergen
中科院分区：
文献类型：
--
作者：
Cao, Zhengwen;Jiang, Heqing;Caro, Juergen
甲烷脱氢芳构化反应（MDA）由于其在甲烷转化为化学品和液体燃料方面的巨大潜力而引起了学术界和工业界的广泛关注。[1]与传统的基于费托合成气（CO+2 H2）技术的液体燃料生产相比，MDA提供了一种简单、直接和经济的从甲烷到芳烃的途径，而没有中间步骤。已经投入了大量的努力来开发合适的催化剂，例如Zn/HZSM-5、[2] Fe/HZSM-5、[3]和Ga/HZSM-5、[4]，并且已经取得了令人鼓舞的进展，特别是在Mo/MCM-22、[5] Mo/HMCM-49、[6]和Mo/HZSM-5上。[2，7]但催化剂结焦失活快、甲烷转化率低等问题仍然存在，阻碍了MDA的工业化。[8]为了克服反应（1）的平衡限制，提出了可以通过氢渗透膜（金属合金、沸石或其它分子筛、质子/电子传导陶瓷）除去所产生的氢。[9]使用Pd涂覆的Nb-Ta膜，在6008 ℃下甲烷转化率可以从3.8%增加到9%;然而，氢的去除导致加速焦化。[9b]热力学上有利的是用反应（2）的氧化MDA取代反应（1）的非氧化MDA。
Methane dehydroaromatization (MDA) is attracting considerable interest from both academia and industry because of its potential in the conversion of methane into chemicals and liquid fuels.[1] Compared to the conventional liquid fuels production based on Fischer–Tropsch technology from syngas (CO+ 2H2), MDA provides a simple, straightforward, and economic pathway from methane to aromatic hydrocarbons without intermediate steps. Intensive efforts have been devoted to the development of suitable catalysts, such as Zn/HZSM-5,[2] Fe/HZSM-5,[3] and Ga/HZSM-5,[4] and encouraging progress has been made, especially on Mo/MCM-22,[5] Mo/HMCM-49,[6] and Mo/HZSM-5.[2, 7] Challenging problems still exist, such as the rapid catalyst deactivation by coke and the limited methane conversion, which hinder the industrialization of MDA.[8] To overcome the equilibrium limitation of Reaction (1), it is proposed that the generated hydrogen can be removed by hydrogen-permeable membranes (metal alloys, zeolite or other molecular sieves, proton/electron conducting ceramics).[9] Using a Pd-coated Nb-Ta membrane, the methane conversion could be increased from 3.8% to 9% at 6008C; however, hydrogen removal resulted in accelerated coking.[9b] Thermodynamically favorable is the substitution of the nonoxidative MDA according to Reaction (1) by the oxidative MDA according to Reaction (2).