Synergistic mechanism between Brønsted acid site and active cerium species in hydride transfer reaction over CeY zeolites

IF 7.2 1区 化学 Q1 CHEMISTRY, APPLIED
Jianhao Jiao , Yucai Qin , Jian Zheng , Yu Hui , Li Zhang , Xionghou Gao , Lijuan Song
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引用次数: 2

Abstract

In this study, cyclohexene was used as a representative of olefin and catalyzed by CeY zeolites in a fixed-bed reactor under mild conditions, and the influence of Ce species in hydride transfer reaction over CeY zeolites was evaluated. CeY zeolites show more excellent hydride transfer properties than HY zeolite. Based on the results of almost identical Brønsted acid properties but not the product distributions for 0.075CeY and 0.075CeY(DC) samples, it should be suggested that the Brønsted acid strength and density are not the deciding factors to the hydride transfer reaction. A unique band at 1442 cm−1 in situ FTIR spectroscopy spectra are assigned to pyridine complexes bonded to a class of active Ce species that could reversibly migrate from the core of SOD cages to its 6-rings mouth towards the supercages. These results provide valuable information that these active Ce species should play a synergistic role with the Brønsted acid sites in enhancing the hydride transfer reaction with a bimolecular mechanism over CeY zeolites.

Abstract Image

CeY沸石氢化物转移反应中Brønsted酸位与活性铈的协同作用机理
本研究以环己烯为代表的烯烃,在固定床反应器中,在温和条件下由CeY沸石催化,考察了Ce种类对CeY沸石氢化物转移反应的影响。CeY分子筛的氢化物转移性能优于HY分子筛。0.075 5cey和0.075 5cey (DC)样品的Brønsted酸性质几乎相同,但产物分布不同,因此可以认为Brønsted酸强度和密度不是氢化物转移反应的决定因素。在1442 cm−1的原位FTIR光谱中,吡啶配合物被分配到一类活性Ce物质上,这些活性Ce物质可以从SOD笼的核心可逆地迁移到超笼的6环口。这些结果提供了有价值的信息,表明这些活性Ce应该与Brønsted酸位协同作用,以双分子机制增强CeY沸石上的氢化物转移反应。
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来源期刊
Journal of Rare Earths
Journal of Rare Earths 化学-应用化学
CiteScore
8.70
自引率
14.30%
发文量
374
审稿时长
1.7 months
期刊介绍: The Journal of Rare Earths reports studies on the 17 rare earth elements. It is a unique English-language learned journal that publishes works on various aspects of basic theory and applied science in the field of rare earths (RE). The journal accepts original high-quality original research papers and review articles with inventive content, and complete experimental data. It represents high academic standards and new progress in the RE field. Due to the advantage of abundant RE resources of China, the research on RE develops very actively, and papers on the latest progress in this field emerge every year. It is not only an important resource in which technicians publish and obtain their latest research results on RE, but also an important way of reflecting the updated progress in RE research field. The Journal of Rare Earths covers all research and application of RE rare earths including spectroscopy, luminescence and phosphors, rare earth catalysis, magnetism and magnetic materials, advanced rare earth materials, RE chemistry & hydrometallurgy, RE metallography & pyrometallurgy, RE new materials, RE solid state physics & solid state chemistry, rare earth applications, RE analysis & test, RE geology & ore dressing, etc.
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Cyclohexene
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