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Direct Conversion of Syngas into Methyl Acetate, Ethanol, and Ethylene by Relay Catalysis via the Intermediate Dimethyl Ether
Author(s) -
Zhou Wei,
Kang Jincan,
Cheng Kang,
He Shun,
Shi Jiaqing,
Zhou Cheng,
Zhang Qinghong,
Chen Junchao,
Peng Luming,
Chen Mingshu,
Wang Ye
Publication year - 2018
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201807113
Subject(s) - dimethyl ether , syngas , chemistry , catalysis , selectivity , ethylene , acetic acid , methanol , oxygenate , inorganic chemistry , organic chemistry
Selective conversion of syngas (CO/H 2 ) into C 2+ oxygenates is a highly attractive but challenging target. Herein, we report the direct conversion of syngas into methyl acetate (MA) by relay catalysis. MA can be formed at a lower temperature (ca. 473 K) using Cu‐Zn‐Al oxide/H‐ZSM‐5 and zeolite mordenite (H‐MOR) catalysts separated by quartz wool (denoted as Cu‐Zn‐Al/H‐ZSM‐5|H‐MOR) and also at higher temperatures (603–643 K) without significant deactivation using spinel‐structured ZnAl 2 O 4 |H‐MOR. The selectivity of MA and acetic acid (AA) reaches 87 % at a CO conversion of 11 % at 643 K. Dimethyl ether (DME) is the key intermediate and the carbonylation of DME results in MA with high selectivity. We found that the relay catalysis using ZnAl 2 O 4 |H‐MOR|ZnAl 2 O 4 gives ethanol as the major product, while ethylene is formed with a layer‐by‐layer ZnAl 2 O 4 |H‐MOR|ZnAl 2 O 4 |H‐MOR combination. Close proximity between ZnAl 2 O 4 and H‐MOR increases ethylene selectivity to 65 %.