Direct Conversion of Syngas into Methyl Acetate,Ethanol, and Ethylene by Relay Catalysis via the Intermediate Dimethyl Ether |
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| Authors: | Wei Zhou Dr Jincan Kang Dr Kang Cheng Shun He Jiaqing Shi Cheng Zhou Prof?Dr Qinghong Zhang Junchao Chen Prof?Dr Luming Peng Prof?Dr Mingshu Chen Prof?Dr Ye Wang |
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| Institution: | 1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China;2. Key Lab of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China |
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| Abstract: | Selective conversion of syngas (CO/H2) into C2+ 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 ZnAl2O4|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 ZnAl2O4|H‐MOR|ZnAl2O4 gives ethanol as the major product, while ethylene is formed with a layer‐by‐layer ZnAl2O4|H‐MOR|ZnAl2O4|H‐MOR combination. Close proximity between ZnAl2O4 and H‐MOR increases ethylene selectivity to 65 %. |
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| Keywords: | C2+ oxygenates C− C coupling heterogeneous catalysis relay catalysis zeolites |
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