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Synergistic mechanism between Brønsted acid site and active cerium species in hydride transfer reaction over CeY zeolites
Journal of Rare Earths ( IF 4.9 ) Pub Date : 2020-08-01 , DOI: 10.1016/j.jre.2020.06.001
Jianhao Jiao , Yucai Qin , Jian Zheng , Yu Hui , Li Zhang , Xionghou Gao , Lijuan Song

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 Bronsted acid properties but not the product distributions for 0.075CeY and 0.075CeY(DC) samples, it should be suggested that the Bronsted 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 Bronsted acid sites in enhancing the hydride transfer reaction with a bimolecular mechanism over CeY zeolites.

中文翻译:

CeY沸石上氢化物转移反应中Brønsted酸位点与活性铈物种之间的协同机制

摘要 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,评价Ce物种在氢化物转移反应中对CeY沸石的影响。CeY沸石显示出比HY沸石更优异的氢化物转移性能。基于几乎相同的布朗斯台德酸性质而不是 0.075CeY 和 0.075CeY(DC) 样品的产物分布的结果,应该表明布朗斯台德酸强度和密度不是氢化物转移反应的决定因素。1442 cm-1 处的独特谱带原位 FTIR 光谱被分配给与一类活性 Ce 物质键合的吡啶配合物,这些 Ce 物质可以从 SOD 笼的核心可逆地迁移到其 6 环口朝向超级笼。
更新日期:2020-08-01
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