Ce3+-掺入HZSM-5作为环己烯水化的高效催化剂，具有丰富的强Brønsted酸位

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-07-13 DOI:10.1016/j.apcata.2025.120451

Hefang Wang , Shijiao Hao , Hui Jiang, Xiaofei Ma, Hashim Khan, Jingwei Liu, Weiqian Qi

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引用次数: 0

摘要

采用湿浸渍法制备了一系列Ce3+掺杂HZSM-5催化剂，用于环己烯水化。XRD, Vacuum-IR， XPS和29Si NMR证实Ce3+成功掺入HZSM-5中。NH3-TPD和Py-IR分析表明，与HZSM-5相比，Ce-HZSM-5催化剂显著提高了强Brønsted酸密度。此外，3.0Ce-HZSM-5的强Brønsted/Lewis酸比是HZSM-5的4倍（9.2 vs 2.3）。结果表明，该催化剂具有良好的催化活性，环己烯转化率为12.7% %，环己醇选择性为99.9% %，经过5次循环后仍保持较高的催化性能。采用原位红外光谱对环己烯水化反应机理进行了研究。结果表明，Ce3+与Si-OH相互作用形成新的强Bronsted酸位点（Si-OH - ce）。该位点能有效促进环己烯的活化，显著提高催化水化性能。

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Ce3+-incorporated HZSM-5 as efficient catalysts with rich-strong Brønsted acid sites for cyclohexene hydration

A series of Ce³⁺ incorporated HZSM-5 catalysts were prepared by wet impregnation method for cyclohexene hydration. XRD, Vacuum-IR, XPS, and ²⁹Si NMR confirmed the successful incorporation of Ce³⁺ into the HZSM-5. NH₃-TPD and Py-IR analyses revealed that Ce-HZSM-5 catalyst significantly increased strong Brønsted acid density compared to HZSM-5. Further, the strong Brønsted/Lewis acid ratio of 3.0Ce-HZSM-5 is 4-fold higher than that of HZSM-5 (9.2 vs 2.3). As a result, the catalyst exhibited excellent activity with 12.7 % conversion of cyclohexene and 99.9 % selectivity to cyclohexanol and maintained high catalytic performance after five cycles. In situ FTIR was used to investigate the cyclohexene hydration reaction mechanism. The results showed that Ce³⁺ interacts with Si–OH to form a new strong Bronsted acid site (Si–OH–Ce). This site can effectively promote the activation of cyclohexene and significantly enhance the catalytic hydration performance.

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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.