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Facile preparation of Ni/Al2O3 catalytic formulations with the aid of cyclodextrin complexes: Towards highly active and robust catalysts for the direct amination of alcohols
Journal of Catalysis ( IF 7.3 ) Pub Date : 2017-11-06 , DOI: 10.1016/j.jcat.2017.10.006
Ajay Tomer , Frédéric Wyrwalski , Cédric Przybylski , Jean-François Paul , Eric Monflier , Marc Pera-Titus , Anne Ponchel

A series of Ni/Al2O3 catalysts with variable Ni loading (2–20 wt%) were prepared by aqueous wet impregnation of a nitrate precursor using native cyclodextrins as metal complex hosts. The impact of β-CD was carefully characterized at different stages of the preparation by a set of complementary techniques including TG-MS analysis, mass spectrometry, X-ray diffraction, temperature-programmed reduction, CO pulse chemisorption, X-ray photoelectron spectroscopy and electron microscopy. It was found that the use of cyclodextrins afforded a much higher Ni dispersion and narrower distribution of Ni particle sizes, as well as a much higher availability of reduced surface Ni species. As a result, the cyclodextrin-assisted catalysts exhibited enhanced catalytic properties in the direct amination of benzyl alcohol with aniline and 1-octanol with ammonia, both operated via the hydrogen borrowing mechanism. Furthermore, the use of cyclodextrins allowed a significant improvement of the robustness of the catalysts by mitigating the nickel leaching during reaction.



中文翻译:

借助环糊精配合物轻松制备Ni / Al 2 O 3催化配方:寻求高活性和强固性的催化剂,用于醇的直接胺化

一系列的Ni / Al 2 O 3通过使用天然环糊精作为金属配合物主体,对硝酸盐前驱物进行湿法浸渍,制备了具有可变Ni负载量(2-20 wt%)的催化剂。通过一系列辅助技术,包括TG-MS分析,质谱,X射线衍射,程序升温还原,CO脉冲化学吸附,X射线光电子能谱和电子显微镜。已经发现,使用环糊精可提供更高的镍分散度和更窄的镍粒度分布,以及更高的还原性表面镍物种可用性。结果,环糊精助催化剂在苯甲醇与苯胺直接氨化和1-辛醇与氨直接氨化中均显示出增强的催化性能,两者均操作通过氢借用机制。此外,环糊精的使用通过减轻反应期间的镍浸出而允许显着改善催化剂的坚固性。

更新日期:2017-11-06
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