Improving the dehydrogenation function and stability of Zn-modified ZSM-5 catalyst in methanol-to-aromatics reaction by Ca addition

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-06-22 DOI:10.1016/j.apcata.2024.119854
Héctor Vicente , Chuncheng Liu , Ana G. Gayubo , Pedro Castaño , Evgeny A. Pidko
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Abstract

Adding Zn to the ZSM-5 zeolite effectively increases the aromatic selectivity in the methanol-to-aromatics (MTA) process. The formation of metal-derived Lewis acid sites promotes the dehydrogenation but at the cost of a rapid deactivation of the catalyst by coke, due to the increased aromatic formation. In this work, we impregnated a Zn-modified catalyst (2 wt%) with variable contents of Ca (0.02 and 0.5 wt%) and evaluated their kinetic behavior in the MTA and ethane dehydrogenation reactions. The results proved the superior performance of the Zn(2)Ca(0.02) catalyst due to a synergistic effect between the two metals. The Ca ions limit coke formation from excessive aromatization, increasing catalyst stability and removing Zn clusters, resulting in a recovery of Brønsted acid sites (BAS) active for the formation of light aromatics. Combining these effects results in a more efficient and viable catalyst for aromatic production from methanol.

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通过添加 Ca 提高 Zn 改性 ZSM-5 催化剂在甲醇制芳烃反应中的脱氢功能和稳定性
在 ZSM-5 沸石中添加锌可有效提高甲醇制芳烃 (MTA) 过程中的芳烃选择性。金属衍生路易斯酸位点的形成促进了脱氢反应,但其代价是由于芳烃的形成增加,催化剂会因焦炭而迅速失活。在这项工作中,我们在 Zn 改性催化剂(2 wt%)中浸渍了不同含量的 Ca(0.02 和 0.5 wt%),并评估了它们在 MTA 和乙烷脱氢反应中的动力学行为。结果表明,Zn(2)Ca(0.02) 催化剂的性能优越,这是由于两种金属之间的协同效应。Ca 离子限制了因过度芳香化而形成的焦炭,提高了催化剂的稳定性,并清除了 Zn 团簇,从而恢复了对轻芳烃形成具有活力的布氏硬度酸位点 (BAS)。将这些作用结合在一起,就能产生一种更高效、更可行的催化剂,用于从甲醇中生产芳烃。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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