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双功能催化剂上通过级联反应由合成气直接合成增值芳烃化学品的研究进展

Recent Advances in Direct Synthesis of Value-Added Aromatic Chemicals from Syngas by Cascade Reactions over Bifunctional Catalysts.

作者信息

Kasipandi Saravanan, Bae Jong Wook

机构信息

School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu-ro, Jangan-gu, Suwon, Gyeonggi-do, 16419, Republic of Korea.

出版信息

Adv Mater. 2019 Aug;31(34):e1803390. doi: 10.1002/adma.201803390. Epub 2019 Feb 15.

Abstract

Value-added aromatic monomers such as benzene, toluene, and xylenes (BTX) are very important building-block chemicals for the production of plastics, polymers, solvents, pesticides, dyes, and adhesives. Syngas-to-aromatics (STA) is a very promising approach for the synthesis of aromatic monomers, and is catalyzed via bifunctional catalysts in a single reactor, wherein methanol/dimethyl ether and/or olefins intermediates formed from syngas on metal components are converted into aromatic monomers exclusively on the HZSM-5 by cascade reactions. Since an optimal Fischer-Tropsch synthesis (FTS) temperature of Fe-based catalysts is very close to an aromatization temperature of HZSM-5, Fe-based catalysts have been frequently used/modified for the synthesis of aromatic monomers from hydrogenation of carbon oxides (CO and CO ). The nature of metal components and amounts of Brönsted acid sites on HZSM-5, and their mesoporosity and intimacy, significantly alter the selectivity for aromatics by tuning BTX distibution and catalyst stability. Although many developments have been achieved regarding the STA process in recent years, no reviews have been published in this flourishing research area over the last two decades. Here, the recent advances and forthcoming challenges in the progress of syngas (CO+H ) chemistry and hydrogenation of CO toward the value-added aromatic monomers through cascade reactions are highlighted.

摘要

增值芳香族单体,如苯、甲苯和二甲苯(BTX),是生产塑料、聚合物、溶剂、农药、染料和粘合剂的非常重要的基础化学品。合成气制芳烃(STA)是一种非常有前景的合成芳香族单体的方法,它在单个反应器中通过双功能催化剂进行催化,其中合成气在金属组分上形成的甲醇/二甲醚和/或烯烃中间体通过级联反应仅在HZSM-5上转化为芳香族单体。由于铁基催化剂的最佳费托合成(FTS)温度与HZSM-5的芳构化温度非常接近,铁基催化剂经常被用于/改性以通过二氧化碳(CO和CO)加氢合成芳香族单体。HZSM-5上金属组分的性质、布朗斯台德酸位的数量及其介孔率和紧密程度,通过调节BTX分布和催化剂稳定性,显著改变对芳烃的选择性。尽管近年来在STA工艺方面已经取得了许多进展,但在过去二十年里,在这个蓬勃发展的研究领域还没有发表过综述。在此,重点介绍了合成气(CO+H)化学以及通过级联反应将CO加氢转化为增值芳香族单体过程中的最新进展和即将面临的挑战。

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