Insight into the coke alleviation pattern over iron-based and boron-modified HZSM-5 bifunctional catalyst for direct CO2 hydrogenation to aromatics

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2024-11-19 DOI:10.1016/j.apcata.2024.120029

Chonghao Chen , Zixin Song , Dianhua Liu

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引用次数: 0

Abstract

Carbon dioxide (CO₂) hydrogenation to aromatics is promising for reducing the burden of petroleum fuels. Herein, iron-based catalyst was mixed with boron modified HZSM-5 with pre-treatment and post-treatment method. The textural, acidic and element distribution properties over zeolite framework and external surface were studied. Combining with characterizations for internal and external coke, the element distribution-acidity-coke-stability relationship over boron-modified zeolite was put forward. Pre-treated zeolite witnessed reduced amount of external and total Brönsted acid sites (BAS) with similar degree, and increase paired Al (Al_pair) fraction in the intersection site, leading to increased aromatics selectivity and reduced coke amount. While boron post-treatment significantly reduced external surface BAS and inhibited formation of condensed external coke. Afterwards, the mechanism of olefins aromatization was studied and found that PT-Z5-B greatly suppressed the overalkylation of light aromatics, thus alleviating the co-deactivation pattern generated by transformation of coke precursors from zeolite to iron-based catalyst.

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铁基和硼改性 HZSM-5 双功能催化剂在二氧化碳直接加氢制芳烃过程中焦炭缓解模式的深入研究

二氧化碳（CO2）加氢制芳烃有望减轻石油燃料的负担。本文采用预处理和后处理方法，将铁基催化剂与硼改性 HZSM-5 混合。研究了沸石框架和外表面的质地、酸性和元素分布特性。结合内部和外部焦炭的表征，提出了硼改性沸石的元素分布-酸性-焦炭-稳定性关系。经预处理的沸石外表面和总布伦斯特酸位点（BAS）的数量减少了，且程度相近，而交叉位点中成对的 Al（Alpair）组分增加了，从而提高了芳烃选择性并减少了焦炭数量。而硼后处理则大大降低了外表面 BAS，抑制了凝结外焦的形成。随后，对烯烃芳构化机理进行了研究，发现 PT-Z5-B 大大抑制了轻芳烃的过烷基化，从而缓解了焦炭前体从沸石转化为铁基催化剂所产生的共失活模式。

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

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.