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Enhanced Friedel-Crafts benzylation activity of bimetallic WSn-KIT-6 catalysts
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-07-10 , DOI: 10.1016/j.jcat.2020.07.001
Rajamanickam Maheswari , Anand Ramanathan , Hongda Zhu , Aline Araújo do Nascimento Araújo , Clint Chapman , Yu Tang , Franklin (Feng) Tao , Bala Subramaniam

A series of W and Sn-containing KIT-6 mesoporous silicates (designated as WxSn5) with similar Sn (~5 wt%) and varying W (x = 3–23 wt%) loadings were prepared by a one-pot hydrothermal synthesis method. No detectable bulk WO3 species were observed for W loading up to 14 wt% with preferential dispersion of WOx species near SnO2 sites. The WxSn5 materials exhibited superior performance for Friedel-Crafts anisole benzylation with intrinsic rate constants for all WxSn5 catalysts being greater than those without Sn. Based on results from DR-UV–Vis, XRD, XPS, EXAFS techniques, we postulate that the WxSn5 materials contain both isolated [WO4]2-/SnO2 and isolated [WO4]2-/SiO2 as active species, with the former being more active. The relative populations of these two highly dispersed species dictate the overall catalyst activity. The intrinsic activities of the WxSn5 catalysts are found to scale linearly with total acidity but are mainly dictated by the Lewis acid sites.



中文翻译:

双金属WSn-KIT-6催化剂的Friedel-Crafts苄基化活性增强

 用一个锅准备了一系列含W和Sn的KIT-6中孔硅酸盐(指定为W x Sn 5),具有相似的Sn(〜5 wt%)和变化的W(x = 3–23 wt%)负载。水热合成法。没有观察到W含量高达14重量%的可检测的大块WO 3物种,其中WO x物种优先分散在SnO 2位点附近。W x Sn 5材料表现出对Friedel-Crafts茴香醚苄基化的优异性能,所有W x Sn 5的固有速率常数催化剂比没有锡的催化剂大。根据DR-UV-Vis,XRD,XPS,EXAFS技术的结果,我们假设W x Sn 5材料包含分离的[WO 4 ] 2- / SnO 2和分离的[WO 4 ] 2- / SiO 2作为活跃的物种,前者更为活跃。这两个高度分散的物种的相对种群决定了整体催化剂活性。发现W x Sn 5催化剂的固有活性与总酸度成线性比例,但主要由路易斯酸位决定。

更新日期:2020-07-26
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