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Sn-Beta zeolite derived from a precursor synthesized via an organotemplate-free route as efficient Lewis acid catalyst
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-02-25 , DOI: 10.1016/j.apcata.2018.02.017
Zhiguo Zhu , Hao Xu , Jingang Jiang , Yejun Guan , Peng Wu

Sn-containing Beta zeolite (Sn-Beta) is an effective solid Lewis acid catalyst useful for a large number of redox reactions. However, it is still a challenging task to prepare Sn-Beta without the usage of organic structure directing agents (OSDAs) and/or fluoride. Considering synthesis cost and the consumption of energy as well as environmental problems, in this study, hierarchical Sn-Beta is successfully prepared via post-synthesis method by incorporating Sn ions into silanol nests of dealuminated Beta zeolite which is synthesized through an OSDA- and fluoride-free route. Prior to deep dealumination, the OSDA-free aluminosilicate Beta is steamed at a mild temperature for a short time (823 K, 30 min), which allows for the effectively stabilizing the Beta framework structure. Then Sn ions are tetrahedrally incorporated into the Beta framework at 773 K under vapor condition via the reaction between the Sn ions and silanol defects derived from the steaming and subsequent acid treatment. The Sn-Beta zeolite thus obtained exhibits better catalytic performances than conventional Sn-Beta-F in the conversion of dihydroxyacetone to ethyl lactate (yield, 89.1% vs. 74.3%) and Baeyer-Villiger oxidation of 2-adamantanone (conversion, 72.3% vs. 58.6%, using H2O2 as the oxidant). The enhanced catalytic performance is predominantly contributed by hierarchical pore channels and the smaller particle size, which greatly enhance mass transfer and lower the apparent reaction activation energy.



中文翻译:

衍生自前体的Sn-Beta沸石通过无有机模板的途径合成为有效的路易斯酸催化剂

含锡的Beta沸石(Sn-Beta)是有效的固体路易斯酸催化剂,可用于大量的氧化还原反应。但是,在不使用有机结构导向剂(OSDA)和/或氟化物的情况下制备Sn-Beta仍然是一项艰巨的任务。考虑到合成成本,能源消耗以及环境问题,本研究成功地通过通过将Sn离子掺入脱铝Beta沸石的硅烷醇巢中的后合成方法,该脱铝Beta沸石是通过无OSDA和无氟化物的路线合成的。在深度脱铝之前,将不含OSDA的铝硅酸盐Beta在温和的温度下蒸短时间(823 K,30分钟),这可以有效地稳定Beta框架结构。然后,在蒸汽条件下,在773 K下,Sn离子以四面体形式通过Sn离子与由蒸制和随后的酸处理引起的硅烷醇缺陷之间的反应。这样获得的Sn-Beta沸石在二羟基丙酮转化为乳酸乙酯(产率,89.1%vs. 74.3%)和2-金刚烷酮的Baeyer-Villiger氧化(转化率,72.3%)方面表现出比常规Sn-Beta-F更好的催化性能。 (使用H 2 O 2作为氧化剂,则为58.6%)。增强的催化性能主要归因于分级的孔道和较小的粒径,这极大地增强了传质并降低了表观反应活化能。

更新日期:2018-02-25
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