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

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2024-11-30 DOI:10.1002/aic.18664

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

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引用次数: 0

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.

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继电催化合成气直接转化为乙酸甲酯：从活性位点的制备到过程控制

由于反应网络复杂，合成气直接和选择性地转化为C2+氧合物具有挑战性。在这里，我们报道了一个强大的从合成气直接合成乙酸甲酯（MA）的接力系统，该系统将CuZnAlOx/H-ZSM-5与用于合成气二甲醚（DME）羰基化的改性H-MOR结合起来。在H-ZSM-5上甲醇脱水制二甲醚，由于二甲醚的平衡产率高，CuZnAlOx上CO的加氢反应明显增强。碱性分子阻断Brönsted酸位或选择性脱铝H-MOR中12元环抑制沸石焦化。此外，240℃以上的反应温度避免了H-MOR 8-MR侧袋内羰基化位点的H2O中毒，进一步有利于催化稳定性。最终，该接力系统提供了75%的MA选择性和13%的醋酸选择性，CO转化率为65%，优于现有的催化剂。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.

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索莱宝

1,3-dimethyl imidazolium chloride

索莱宝

1,3-dimethyl imidazolium chloride