Synthesis of reaction‐adapted zeolites as methanol-to-olefins catalysts with mimics of reaction intermediates as organic structure‐directing agents

催化作用 化学 甲醇 反应中间体 反应机理 乙烯 沸石 组合化学 反应条件 有机化学
作者
Chengeng Li,Cecilia Paris,Joaquín Martínez‐Triguero,Mercedes Boronat,Manuel Moliner,Avelino Corma
出处
期刊:Nature Catalysis [Nature Portfolio]
卷期号:1 (7): 547-554 被引量:123
标识
DOI:10.1038/s41929-018-0104-7
摘要

Catalysis with enzymes and zeolites have in common the presence of well-defined single active sites and pockets/cavities where the reaction transition states can be stabilized by longer-range interactions. We show here that for a complex reaction, such as the conversion of methanol-to-olefins (MTO), it is possible to synthesize reaction-adapted zeolites by using mimics of the key molecular species involved in the MTO mechanism. Effort has focused on the intermediates of the paring mechanism because the paring is less favoured energetically than the side-chain route. All the organic structure-directing agents based on intermediate mimics crystallize cage-based small-pore zeolitic materials, all of them capable of performing the MTO reaction. Among the zeolites obtained, RTH favours the whole reaction steps following the paring route and gives the highest propylene/ethylene ratio compared to traditional CHA-related zeolites (3.07 and 0.86, respectively). Methanol-to-olefins (MTO) conversion over zeolites is a promising route for the production of light olefins. Now, Corma and co-workers show that using mimics of reaction intermediates as structure-directing agents allows the synthesis of highly selective zeolite MTO-catalysts.
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