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择形沸石通过乙烯酮中间体促进合成气生成乙烯。

Shape-Selective Zeolites Promote Ethylene Formation from Syngas via a Ketene Intermediate.

作者信息

Jiao Feng, Pan Xiulian, Gong Ke, Chen Yuxiang, Li Gen, Bao Xinhe

机构信息

State Key Laboratory of Catalysis, National Laboratory for Clean Energy, 2011-Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.

University of Chinese Academy of Sciences, Beijing, 100049, China.

出版信息

Angew Chem Int Ed Engl. 2018 Apr 16;57(17):4692-4696. doi: 10.1002/anie.201801397. Epub 2018 Mar 23.

Abstract

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 -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.

摘要

费托合成(FTS)进行的合成气转化的特点是碳氢化合物产物分布广泛,碳原子数从1到几个不等。本文报道,通过采用ZnCrO-丝光沸石(MOR)的氧化物-沸石(OX-ZEO)催化剂概念,产物选择性可有效导向乙烯。在CO转化率为26%时,仅乙烯的选择性在其他碳氢化合物中就高达73%。该选择性显著高于任何其他直接合成气转化或多步甲醇制烯烃转化过程中获得的选择性。这种高选择性途径是通过乙烯酮中间体在MOR的8元环(8MR)侧袋内的催化位点上实现的,而不是通过8MR或12MR通道中的甲醇。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。

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