Effect of Co occurrence state on catalytic and coke resistance performance of SAPO-34 in MTO reaction

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-04-05 Epub Date: 2025-02-18 DOI:10.1016/j.apcata.2025.120171
Ning Li , Jingbo Li , Jianqiao Zhao , Huili Liu , Jiayun Tang , Ruizhi Chu , Xianliang Meng , Weisong Li , Xiao Li
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Abstract

This paper prepared two different occurrence state of cobalt-modified SAPO-34 by impregnation and in situ synthesis, investigating effects on methanol-to-olefin reaction performance. The results showed that the Co modification improved the pore structure, increased the weak acid concentration, and extended the catalytic lifetime of SAPO-34. Among them, the framework-substituted Co-based zeolite has higher olefin selectivity and longer life than SAPO-34 with metal Co on the surface. Besides, the key coke precursors like methyl-substituted benzenes were preferentially deposited in micropores and strong acid sites, and significantly promote the generation of condensed ring aromatic hydrocarbons. While the relatively large mesopore volume and slightly lower strong acid concentration of the framework-substituted Co-based zeolite can synergize reduce the formation rate of coke and inhibit the formation of polycyclic aromatic hydrocarbons, thus improving SAPO-34's anti-coking performance. This revelation sparked a novel concept aimed at enhancing the anti-coking capabilities of metal-based zeolites.
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Co存在状态对MTO反应中SAPO-34催化性能和抗焦性能的影响
本文采用浸渍法和原位合成法制备了两种不同赋存状态的钴改性SAPO-34,考察了其对甲醇-烯烃反应性能的影响。结果表明,Co改性改善了SAPO-34的孔结构,提高了弱酸浓度,延长了SAPO-34的催化寿命。其中,框架取代的Co基分子筛比表面含有金属Co的SAPO-34分子筛具有更高的烯烃选择性和更长的寿命。此外,甲基取代苯等关键焦炭前体优先沉积在微孔和强酸位点,并显著促进缩合环芳烃的生成。而骨架取代co基沸石较大的介孔体积和稍低的强酸浓度可以协同降低焦炭的生成速率,抑制多环芳烃的生成,从而提高SAPO-34的抗焦化性能。这一发现引发了一个旨在提高金属基沸石抗结焦能力的新概念。
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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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