Palladium with spindle-like nitrogen ligand supported on mesoporous silica SBA-15: A tailored catalyst for homocoupling of alkynes and Suzuki coupling

Palladium with spindle-like nitrogen ligand supported on mesoporous silica SBA-15: A tailored catalyst for homocoupling of alkynes and Suzuki coupling
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介孔二氧化硅 SBA-15 上负载的具有纺锤状氮配体的钯:用于炔烃自偶联和铃木偶联的定制催化剂

DOI:
10.1016/j.micromeso.2011.08.010
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发表时间:
2012-01
影响因子:
5.2
通讯作者:
Qiaosheng Pu
Qiaosheng Pu
中科院分区:
材料科学2区
文献类型:
--
作者:
Hongling Li;Min Yang;Qiaosheng Pu

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成功制备了具有纺锤状氮供体基团的介孔二氧化硅SBA-15负载的钯1,4-二氮杂双环[2.2.2]辛烷,并将其应用于末端炔烃的自偶联。该催化剂对带有各种取代基的末端炔烃表现出非常高的活性,产率在70%至94%之间,并且具有以空气作为氧化剂的显着优势。它还表现出良好的可重复使用性,可以通过过滤和洗涤轻松回收,并且重复使用至少五次,几乎没有明显的催化性能损失。此外,它还被证明是一种有效且空气稳定的多相催化剂,适用于芳基卤化物(X=I,Br)与芳基硼酸的 Suzuki 偶联。采用元素分析、X射线光电子能谱、高分辨率透射电子显微镜、氮气物理吸附、Brunauer-Emmett-Teller法和X射线粉末衍射等方法对催化剂进行了系统表征。分析表明,在固定过程中保留了材料的介孔结构。
A mesoporous silica SBA-15-supported palladium with spindle-like nitrogen donor groups, 1,4-diaza-bicyclo[2.2.2]octane, has been successfully prepared and applied for homocoupling of terminal alkynes. The catalyst exhibited very high activity for terminal alkynes carrying various substitution groups, yields ranging from 70% to 94%, with a significant advantage that air acted as the oxidant. It also showed good reusability, could be easily recovered through filtration and washing, and reused at least five times with virtually no evident loss of catalytic performance. Furthermore, it was also proved to be an effective and air-stable heterogeneous catalyst for Suzuki coupling of aryl halides (X=I, Br) with arylboronic acids. The catalyst was systematically characterized by elemental analysis, X-ray photoelectron spectroscopy, high-resolution transmission electron microscope, nitrogen physical adsorption, Brunauer–Emmett–Teller method and X-ray powder diffraction. The analyses indicated that the mesoporous structure of the materials was retained during the immobilization process.
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