Synthesis of reaction-adapted zeolites as methanol-to-olefins catalysts with mimics of reaction intermediates as organic structure-directing agents
Synthesis of reaction-adapted zeolites as methanol-to-olefins catalysts with mimics of reaction intermediates as organic structure-directing agents
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DOI：
10.1038/s41929-018-0104-7
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发表时间：
2018-07-01
期刊：
影响因子：
37.8
通讯作者：
Corma, Avelino
中科院分区：
文献类型：
--
作者：
Li, Chengeng;Paris, Cecilia;Corma, Avelino
酶和沸石的催化作用都存在明确的单一活性位点和口袋/空腔，其中反应过渡态可以通过长程相互作用来稳定。我们在这里表明，对于一个复杂的反应，如甲醇转化为烯烃（MTO），它是可能的合成反应适应沸石通过使用模拟的关键分子物种参与的MTO机制。努力集中在配对机制的中间体，因为配对比侧链路线在能量上更不受欢迎。所有基于中间体模拟物的有机结构导向剂使笼基小孔沸石材料结晶，它们都能够进行MTO反应。在所获得的沸石中，RTH有利于遵循配对路线的整个反应步骤，并且与传统的CHA相关沸石（分别为3.07和0.86）相比，得到最高的丙烯/乙烯比。
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).