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Catalysis with chemically modified mesoporous silicas: Stability of the mesostructure under Suzuki-Miyaura reaction conditions

机译:化学修饰的介孔二氧化硅的催化:Suzuki-Miyaura反应条件下介孔结构的稳定性

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摘要

The use of functionalized mesoporous silicas such as SBA-15 and MCM-41 as supports for Pd catalysis has become increasingly common, notably in important reactions such as the Suzuki-Miyaura reaction. However the analysis of the structural consequences of exposure to these harsh reaction conditions is not nearly as common. We report herein a study of the effect of the Suzuki-Miyaura reaction conditions on the mesoporous material, and on the catalytic activity of the resulting material. Although it has been determined that aqueous base is highly detrimental to the structure of the material, the boric acid produced during the actual coupling reaction has a significant protective effect on the material. This protective effect can be mimicked by the addition of exogenous boric acid to the reaction medium. The use of aluminum-doped material provides an additional protective effect that is not dependent on the presence of boric acid. Finally, we demonstrate conclusively that access to the pores is essential for catalysis, since loss of mesoporosity is coincident with loss of catalytic activity.
机译:使用官能化的介孔二氧化硅(例如SBA-15和MCM-41)作为Pd催化的载体已变得越来越普遍,特别是在重要的反应(例如Suzuki-Miyaura反应)中。然而,对暴露于这些苛刻反应条件下的结构后果的分析并不普遍。我们在此报道了对铃木-宫浦反应条件对介孔材料的影响以及对所得材料的催化活性的研究。尽管已经确定碱水溶液对材料的结构非常有害,但是在实际的偶联反应过程中产生的硼酸对材料具有显着的保护作用。可以通过向反应介质中添加外源硼酸来模仿这种保护作用。掺杂铝的材料的使用提供了附加的保护作用,该保护作用不依赖于硼酸的存在。最后,我们最终证明,进入孔对于催化至关重要,因为中孔性的丧失与催化活性的丧失是同时发生的。

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