Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control

Suhan Liu; Gongli Wu; Yuqing Chen; Yaoyao Han; Mingchao Zhang; Jincan Kang; Min Tang; Krijn P. de Jong; Qinghong Zhang; Ye Wang; Kang Cheng

doi:10.1002/aic.18664

Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control

Suhan Liu, Gongli Wu, Yuqing Chen, Yaoyao Han, Mingchao Zhang, Jincan Kang, Min Tang^*, Krijn P. de Jong, Qinghong Zhang, Ye Wang, Kang Cheng^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The direct and selective conversion of syngas into C₂₊ oxygenates is challenging due to the complex reaction network. Here, we report a robust relay system for the direct synthesis of methyl acetate (MA) from syngas, which combines CuZnAlO_x/H-ZSM-5 for syngas to dimethyl ether (DME) with modified H-MOR for DME carbonylation. The dehydration of methanol to DME on H-ZSM-5 significantly enhanced the hydrogenation of CO on CuZnAlO_x, because of high DME equilibrium yields. Blocking of Brönsted acid sites with basic molecules or selective dealumination of 12-membered rings in H-MOR suppressed the zeolite coking. Besides, reaction temperatures above 240°C avoided H₂O poisoning of carbonylation sites inside 8-MR side pockets of H-MOR, further benefiting the catalytic stability. Eventually, this relay system provided a high MA selectivity of 75% and an acetic acid selectivity of 13% at a CO conversion of 65%, outperforming reported catalysts.

Original language	English
Journal	AICHE Journal
DOIs	https://doi.org/10.1002/aic.18664
Publication status	E-pub ahead of print - 30 Nov 2024

Keywords

C–C coupling
proximity
relay catalysis
syngas
zeolites

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@article{68a6a58f3cc24bb096e4c1ebe0b6e753,

title = "Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control",

abstract = "The direct and selective conversion of syngas into C2+ oxygenates is challenging due to the complex reaction network. Here, we report a robust relay system for the direct synthesis of methyl acetate (MA) from syngas, which combines CuZnAlOx/H-ZSM-5 for syngas to dimethyl ether (DME) with modified H-MOR for DME carbonylation. The dehydration of methanol to DME on H-ZSM-5 significantly enhanced the hydrogenation of CO on CuZnAlOx, because of high DME equilibrium yields. Blocking of Br{\"o}nsted acid sites with basic molecules or selective dealumination of 12-membered rings in H-MOR suppressed the zeolite coking. Besides, reaction temperatures above 240°C avoided H2O poisoning of carbonylation sites inside 8-MR side pockets of H-MOR, further benefiting the catalytic stability. Eventually, this relay system provided a high MA selectivity of 75% and an acetic acid selectivity of 13% at a CO conversion of 65%, outperforming reported catalysts.",

keywords = "C–C coupling, proximity, relay catalysis, syngas, zeolites",

author = "Suhan Liu and Gongli Wu and Yuqing Chen and Yaoyao Han and Mingchao Zhang and Jincan Kang and Min Tang and {de Jong}, {Krijn P.} and Qinghong Zhang and Ye Wang and Kang Cheng",

note = "Publisher Copyright: {\textcopyright} 2024 American Institute of Chemical Engineers.",

year = "2024",

month = nov,

day = "30",

doi = "10.1002/aic.18664",

language = "English",

journal = "AICHE Journal",

issn = "0001-1541",

publisher = "American Institute of Chemical Engineers",

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TY - JOUR

T1 - Direct conversion of syngas into methyl acetate by relay catalysis

T2 - From fabrication of active sites to process control

AU - Liu, Suhan

AU - Wu, Gongli

AU - Chen, Yuqing

AU - Han, Yaoyao

AU - Zhang, Mingchao

AU - Kang, Jincan

AU - Tang, Min

AU - de Jong, Krijn P.

AU - Zhang, Qinghong

AU - Wang, Ye

AU - Cheng, Kang

PY - 2024/11/30

Y1 - 2024/11/30

N2 - The direct and selective conversion of syngas into C2+ oxygenates is challenging due to the complex reaction network. Here, we report a robust relay system for the direct synthesis of methyl acetate (MA) from syngas, which combines CuZnAlOx/H-ZSM-5 for syngas to dimethyl ether (DME) with modified H-MOR for DME carbonylation. The dehydration of methanol to DME on H-ZSM-5 significantly enhanced the hydrogenation of CO on CuZnAlOx, because of high DME equilibrium yields. Blocking of Brönsted acid sites with basic molecules or selective dealumination of 12-membered rings in H-MOR suppressed the zeolite coking. Besides, reaction temperatures above 240°C avoided H2O poisoning of carbonylation sites inside 8-MR side pockets of H-MOR, further benefiting the catalytic stability. Eventually, this relay system provided a high MA selectivity of 75% and an acetic acid selectivity of 13% at a CO conversion of 65%, outperforming reported catalysts.

AB - The direct and selective conversion of syngas into C2+ oxygenates is challenging due to the complex reaction network. Here, we report a robust relay system for the direct synthesis of methyl acetate (MA) from syngas, which combines CuZnAlOx/H-ZSM-5 for syngas to dimethyl ether (DME) with modified H-MOR for DME carbonylation. The dehydration of methanol to DME on H-ZSM-5 significantly enhanced the hydrogenation of CO on CuZnAlOx, because of high DME equilibrium yields. Blocking of Brönsted acid sites with basic molecules or selective dealumination of 12-membered rings in H-MOR suppressed the zeolite coking. Besides, reaction temperatures above 240°C avoided H2O poisoning of carbonylation sites inside 8-MR side pockets of H-MOR, further benefiting the catalytic stability. Eventually, this relay system provided a high MA selectivity of 75% and an acetic acid selectivity of 13% at a CO conversion of 65%, outperforming reported catalysts.

KW - C–C coupling

KW - proximity

KW - relay catalysis

KW - syngas

KW - zeolites

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U2 - 10.1002/aic.18664

DO - 10.1002/aic.18664

M3 - Article

AN - SCOPUS:85210565788

SN - 0001-1541

JO - AICHE Journal

JF - AICHE Journal

ER -

Direct conversion of syngas into methyl acetate by relay catalysis: From fabrication of active sites to process control

Abstract

Keywords

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