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Core-shell Fe3O4@SiO2@HNbMoO6 nanocomposites : new magnetically recyclable solid acid for heterogeneous catalysis

机译:核-壳型Fe3O4 @ SiO2 @ HNbMoO6纳米复合材料:用于多相催化的新型可磁循环利用的固体酸

摘要

A new type of magnetically recyclable solid acid catalyst was designed and retro-synthesized via a two-step template method. Magnetic Fe3O4 cores were synthesized by a solvothermal approach, and then coated with a silica layer by a sol-gel process in order to improve their stability in acid environments. HNbMoO6 nanosheets used as outer shell precursors were obtained by exfoliating a layered tri-rutile transition metal oxide (LiNbMoO6) via proton exchange and intercalation of tetrabutylammonium cations. Negatively charged nanosheets were assembled upon the Fe3O4@SiO2 particles using poly(diallyldimethylammonium chloride) as an opposite polyelectrolyte via a layer-by-layer sequential adsorption process. Protonation of the outer layer was realized by acid exchange treatment. The protonated core-shell nanocomposites showed effective catalytic properties for Friedel-Crafts alkylation reaction and high magnetic recyclability. These results highlight that the rational design and controllable synthesis of multifunctional catalysts is a promising strategy in "green chemistry" and "green technologies".
机译:设计了一种新型的可磁循环利用的固体酸催化剂,并通过两步模板法进行了逆向合成。通过溶剂热法合成了Fe3O4磁性核,然后通过溶胶-凝胶工艺涂覆了二氧化硅层,以提高其在酸性环境中的稳定性。 HNbMoO6纳米片用作外壳前体是通过质子交换和四丁基铵阳离子的嵌入使层状三金红石过渡金属氧化物(LiNbMoO6)剥落而获得的。使用聚(二烯丙基二甲基氯化铵)作为相反的聚电解质,通过逐层顺序吸附工艺将带负电的纳米片组装在Fe3O4 @ SiO2颗粒上。通过酸交换处理实现外层的质子化。质子化的核-壳纳米复合材料对弗瑞德-克来福特烷基化反应显示出有效的催化性能,并具有较高的磁可循环性。这些结果表明,多功能催化剂的合理设计和可控合成是“绿色化学”和“绿色技术”中一种有前途的策略。

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