Shape‐Selective Zeolites Promote Ethylene Formation from Syngas via a Ketene Intermediate,Angewandte Chemie International Edition

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Shape‐Selective Zeolites Promote Ethylene Formation from Syngas via a Ketene Intermediate
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-03-23 , DOI: 10.1002/anie.201801397
Feng Jiao _{1,

2} , Xiulian Pan ₁ , Ke Gong _{1,

2} , Yuxiang Chen _{1,

2} , Gen Li _{1,

2} , Xinhe Bao ₁

Affiliation

Syngas conversion by Fischer–Tropsch synthesis (FTS) is characterized by a wide distribution of hydrocarbon products ranging from one to a few carbon atoms. Reported here is that the product selectivity is effectively steered toward ethylene by employing the oxide‐zeolite (OX‐ZEO) catalyst concept with ZnCrO_x‐mordenite (MOR). The selectivity of ethylene alone reaches as high as 73 % among other hydrocarbons at a 26 % CO conversion. This selectivity is significantly higher than those obtained in any other direct syngas conversion or the multistep process methanol‐to‐olefin conversion. This highly selective pathway is realized over the catalytic sites within the 8‐membered ring (8MR) side pockets of MOR via a ketene intermediate rather than methanol in the 8MR or 12MR channels. This study provides substantive evidence for a new type of syngas chemistry with ketene as the key reaction intermediate and enables extraordinary ethylene selectivity within the OX‐ZEO catalyst framework.

中文翻译：

择形沸石促进合成气通过丁烯中间产物形成乙烯

费-托合成（FTS）进行的合成气转化的特征是烃产品分布范围很广，从一个到几个碳原子不等。此处报道的是，通过将氧化物沸石（OX-ZEO）催化剂概念与ZnCrO _x结合使用，可以有效地将产物的选择性转向乙烯丝光沸石（MOR）。在其他烃类中，仅以26％的CO转化率，乙烯的选择性就高达73％。该选择性显着高于任何其他直接合成气转化或多步法甲醇制烯烃转化所获得的选择性。这种高选择性的途径是通过乙烯酮中间体而不是甲醇通过8MR或12MR通道在MOR的8元环（8MR）侧袋内的催化位点上实现的。这项研究为以乙烯酮为关键反应中间体的新型合成气化学提供了实质性证据，并在OX-ZEO催化剂框架内实现了非凡的乙烯选择性。

更新日期：2018-03-23

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