In:
Angewandte Chemie, Wiley, Vol. 130, No. 37 ( 2018-09-10), p. 12188-12192
Abstract:
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 %.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v130.37
DOI:
10.1002/ange.201807113
Language:
English
Publisher:
Wiley
Publication Date:
2018
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