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Mechanism of tetralin conversion on zeolites for the production of benzene derivatives
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2020-06-09 , DOI: 10.1039/d0re00128g
Kazuki Nakajima 1, 2, 3, 4 , Satoshi Suganuma 1, 2, 3, 4 , Etsushi Tsuji 1, 2, 3, 4 , Naonobu Katada 1, 2, 3, 4
Affiliation  

Ring-opening of tetralin, which is produced by partial dehydrogenation of naphthalene, was catalyzed by various zeolites. Influences of acidity and textural properties of the zeolites on the activity and selectivity were studied in the reactions of not only tetralin but also butylbenzene and indane as the intermediate models in tetralin conversion. The *BEA zeolite exhibited higher conversion and selectivity to benzene and its derivatives (butylbenzene, toluene, xylenes and ethylbenzene) than the other framework type zeolites. The simultaneous cracking of butylbenzene principally produced benzene. The reaction rate in the ring-opening of tetralin was considerably high on strong Brønsted acid sites in the 12-ring of the *BEA zeolite. The amount of Brønsted acid sites on the *BEA zeolite increased the tetralin conversion but did not affect the selectivity to the products. In tetralin conversion, MOR and FAU zeolites formed more methylindane and naphthalene as by-products, respectively. Methylindane was produced on weak Brønsted acid sites through ring-contraction of tetralin, and naphthalene was formed on Lewis acid sites through dehydrogenation. The influences of the reaction conditions on the catalytic activity in tetralin conversion were also investigated. The contact time increased the conversion, but hardly affected the selectivities to the products. The total pressure also improved the catalytic activity. The pressurized hydrogen decreased the selectivity for methylindane, while it increased for benzene and its derivatives. At 573 K, the selectivities to benzene and its derivatives were high, but the reaction temperature increased the selectivity to the by-products.

中文翻译:

沸石上四氢萘转化机理以生产苯衍生物

由萘的部分脱氢反应制得的四氢萘开环被各种沸石催化。研究了沸石的酸度和质构性质对沸石活性和选择性的影响,不仅以四氢化萘,还以丁苯和茚满作为四氢化萘转化的中间模型。* BEA沸石对苯及其衍生物(丁基​​苯,甲苯,二甲苯和乙苯)的转化率和选择性高于其他骨架型沸石。丁基苯的同时裂化主要产生苯。在* BEA沸石12环的强布朗斯台德酸位点上,四氢化萘开环的反应速率非常高。* BEA沸石上的布朗斯台德酸位点数量增加了四氢化萘的转化率,但不影响产物的选择性。在四氢化萘转化中,MOR和FAU沸石分别形成更多的甲基茚满和萘作为副产物。通过四氢萘的环缩合,在弱布朗斯台德酸位上生成甲基茚满,并通过脱氢在路易斯酸位上形成萘。还研究了反应条件对四氢萘转化催化活性的影响。接触时间增加了转化率,但几乎不影响产物的选择性。总压力也提高了催化活性。加压的氢气降低了对甲基茚满的选择性,同时提高了对苯及其衍生物的选择性。在573 K,
更新日期:2020-06-30
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