Mechanism of the Catalytic Conversion of Methanol to Hydrocarbons
Mechanism of the Catalytic Conversion of Methanol to Hydrocarbons
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DOI：
10.1021/cs3006583
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发表时间：
2013-01-01
期刊：
影响因子：
12.9
通讯作者：
Bhan, Aditya
中科院分区：
文献类型：
--
作者：
Ilias, Samia;Bhan, Aditya
在酸性沸石上甲醇制烃（MTH）催化反应中发现的基于芳烃和烯烃的双重催化循环为合理化这一复杂化学的结构功能关系提供了新的背景。这一观点探讨了六个主要的化学物质参与的碳氢化合物池机制MTH-烯烃甲基化，烯烃裂解，氢转移，环化，芳香族甲基化，和芳香族脱烷基化的重点是什么是已知的速率和机制，这些化学物质。目前对MTH的机理理解将结构功能关系限制于沸石骨架对烃库的身份和所得产物选择性的影响。我们强调需要评估MTH中沸石结构的后果，在实验测得的速率和活化障碍的个别反应步骤和在双烯烃和芳烃催化循环内的物种偏好，以改变其相对传播。在没有单独的反应速率，我们建议使用乙烯/异丁烷的选择性作为一种措施来描述的芳香族和烯烃为基础的循环的传播的相对速率。
The discovery of the dual aromatic- and olefin-based catalytic cycles in methanol-to-hydrocarbons (MTH) catalysis on acid zeolites has given a new context for rationalizing structure function relationships for this complex chemistry. This perspective examines six major chemistries involved in the hydrocarbon pool mechanism for MTH-olefin methylation, olefin cracking, hydrogen transfer, cyclization, aromatic methylation, and aromatic dealkylation-with a focus on what is known about the rate and mechanism of these chemistries. The current mechanistic understanding of MTH limits structure function relationships to the effect of the zeolite framework on the identity of the hydrocarbon pool and the resulting product selectivity. We emphasize the need for assessing the consequences of zeolite structure in MTH in terms of experimentally measured rates and activation barriers for individual reaction steps and in terms of speciation preferences within the dual olefin-and aromatic-catalytic cycles to alter their relative propagation. In the absence of individual reaction rates, we propose using ethene/isobutane selectivity as a measure to describe the relative rates of propagation for the aromatic- and olefin-based cycles.