Highly selective oxidation of amines to imines by Mn2O3 catalyst under eco-friendly conditions  

作　　者：Fushan Chen Tao Yang Songlin Zhao Taotao Jiang Lu Yu Houfeng Xiong Chuankun Guo Yufang Rao Yan Liu Liu Liu Jian Zhou Pengxiang Tu Jun Ni Qunfeng Zhang Xiaonian Li 

机构地区：[1]Industrial Catalysis Institute of Zhejiang University of Technology,Hangzhou 310014,China [2]Jiangxi Province Engineering Research Center of Ecological Chemical Industry,Jiujiang University,Jiujiang 332005,China [3]School of Pharmaceutical and Chemical Engineering,Taizhou University,Taizhou 318000,China

出　　处：《Chinese Chemical Letters》2019年第12期2282-2286,共5页中国化学快报（英文版）

基　　金：Financial support from the National Natural Science Foundation of China (NSFC,Nos.21776258,21476207,91534113,21406199, 21566013,21875220);Program from Science and Technology Department of Zhejiang Province (Nos.2015C31042, LY17B060006);Education Science Planning Project of Jiangxi Province (No.18YB243);Natural Science Foundation of Jiangxi Province (No.20181BAB216032)

摘　　要：Enhancing the selectivity of imines for the oxidative self-coupling of primary amines was found to be challenging in the heterogeneous catalysis.Three different manganese oxides(M-3,M-4,M-5) were synthesized by controlling the calcination temperature using a simple template-free oxalate route.The prepared manganese oxides were systematically characterized using XRD,N2 sorption,SEM,TEM,XPS,H2-TPR techniques.M-4 gave 96.2% selectivity of imine at 100% conversion of benzylamine,which was far more superior than other existing protocols.Mn^3+/Mn^4+ ratio was found to affect the selectivity of the imines.The probable reaction pathway for amines oxidation catalyzed by manganese oxides was proposed for the first time.Enhancing the selectivity of imines for the oxidative self-coupling of primary amines was found to be challenging in the heterogeneous catalysis.Three different manganese oxides（M-3,M-4,M-5） were synthesized by controlling the calcination temperature using a simple template-free oxalate route.The prepared manganese oxides were systematically characterized using XRD,N2 sorption,SEM,TEM,XPS,H2-TPR techniques.M-4 gave 96.2% selectivity of imine at 100% conversion of benzylamine,which was far more superior than other existing protocols.Mn3+/Mn4+ ratio was found to affect the selectivity of the imines.The probable reaction pathway for amines oxidation catalyzed by manganese oxides was proposed for the first time.

关 键 词：Oxalate route MN2O3 Self-coupling of amines Heterogeneous catalysis Aerobic oxidation 

分 类 号：O643.36[理学—物理化学]