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利用氯甲基吡啶与咪唑反应制备了一系列含吡啶取代咪唑L1～L5,考察了所得咪唑衍生物与钌化合物在碱性条件下原位形成的氮杂卡宾钌络合物对苯胺与醇氢转移反应的催化活性.研究了碱的种类、钌前体、温度等对反应的影响,结果表明RuCl3 H2O/1-(2-吡啶甲基)-3-甲基碘化咪唑(L3)/KOH催化体系在185℃时对苯胺与乙二醇反应的催化活性较高,选择性生成N-羟乙基苯胺,TON(单位活性转化的底物分数)可达2130.此外,还考察了RuCl3 H2O/L3/KOH催化体系对苯胺与丁醇、环己醇、异丙醇、苯甲醇反应的催化性能.在催化剂作用下,醇与苯胺可形成亚胺及仲胺,伯醇可以自氢转移反应形成酯,反应产物的结构及选择性取决于醇的结构及反应条件.
A series of pyridine-substituted imidazoles L1 ~ L5 were prepared by the reaction of chloromethylpyridine with imidazole. The effects of azidocarpin ruthenium complexes formed by in-situ formation of imidazole derivatives and ruthenium compounds on aniline and alcohol hydrogens The catalytic activity of the transfer reaction was investigated. The effects of the kind of base, ruthenium precursor and temperature on the reaction were studied. The results showed that RuCl3 H2O / 1- (2-picolyl) -3-methylimidazolium iodide Catalytic system at 185 ° C for aniline and ethylene glycol higher catalytic activity, the selective generation of N-hydroxyethyl aniline, TON (unit activity conversion substrate fraction) up to 2130. In addition, RuCl3 H2O / L3 / KOH catalytic system for the reaction of aniline with butanol, cyclohexanol, isopropanol, benzyl alcohol.At the catalyst, alcohol and aniline can form imine and secondary amine, the primary alcohol can be transferred from the hydrogen reaction Ester formation, the structure and selectivity of the reaction product depends on the structure of the alcohol and the reaction conditions.