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Additive-free aerobic oxidative dehydrogenation of N-heterocycles under catalysis by NiMn layered hydroxide compounds
Journal of Catalysis ( IF 6.5 ) Pub Date : 2018-03-03 , DOI: 10.1016/j.jcat.2018.01.030
Weiyou Zhou , Qianyun Tao , Fu'an Sun , Xinbai Cao , Junfeng Qian , Jie Xu , Mingyang He , Qun Chen , Jianliang Xiao

NiMn layered hydroxide compounds have been found to be efficient catalysts for the oxidative dehydrogenation of N-heterocycles by molecular oxygen under mild conditions. Various tetrahydroquinoline derivatives and some other N-heterocycles have been found to be tolerated by the catalytic system. A synergistic effect between Ni and Mn has been observed in the reaction. A kinetic study concluded that the dehydrogenation of 1,2,3,4-tetrahydroquinoline is a first-order reaction, and an apparent activation energy of 113 kJ/mol has been obtained. A probable reaction mechanism comprising an imine intermediate has been proposed according to the obtained results and XPS analysis. The key catalytic site for the dehydrogenation is thought to be Mn3+, which could be stabilized by Ni2+ in the hydrotalcite structure.



中文翻译:

NiMn层状氢氧化物催化下N杂环的无添加剂好氧氧化脱氢

已发现NiMn层状氢氧化物是在温和条件下通过分子氧对N-杂环进行氧化脱氢的有效催化剂。已经发现各种四氢喹啉衍生物和一些其他N-杂环可被催化体系所耐受。在反应中已经观察到Ni和Mn之间的协同作用。动力学研究得出1,2,3,4-四氢喹啉的脱氢反应是一级反应,表观活化能为113 kJ / mol。根据获得的结果和XPS分析,提出了一种可能的包含亚胺中间体的反应机理。认为脱氢的关键催化位点是Mn 3+,可以通过Ni 2+使其稳定。 在水滑石结构中。

更新日期:2018-03-03
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