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

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION(2018)

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摘要
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 ZnCrOx-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.
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关键词
Ethylene,heterogeneous catalysis,solid-state structures,syngas,zeolites
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