负载型铜原位液相催化胺类化合物的N-甲基化反应研究  

N-Methylation of Amine-Based Compounds by Supported Cu In-Situ Liquid Phase

作　　者：戴玉玉 洪学立 沈纪达 张骏 王亚权[1] 严新焕 DAI Yuyu;HONG Xueli;SHEN Jida;ZHANG Jun;WANG Yaquan;YAN Xinhuan*(School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;College of Chemical Engineering,Zhejiang University of Technology,Hangzhou,Zhejiang 310014,China;Zhejiang Alpha Chemical Technology Co.,Ltd.,Jiaxing,Zhejiang 314304,China)

机构地区：[1]天津大学化工学院,天津300072 [2]浙江工业大学化学工程学院,浙江杭州310014 [3]浙江阿尔法化工科技有限公司,浙江嘉兴314304

出　　处：《浙江化工》2024年第12期23-31,共9页Zhejiang Chemical Industry

基　　金：国家重点研发计划(2017YFC0210901);国家自然科学基金项目(52103272);浙江省自然科学基金项目(LQ21E030004)。

摘　　要：甲醇作为碳源用于原位液相催化胺类化合物的N-甲基化,是一种有效且环保的方法,开发高效的非贵金属催化剂是解决甲醇脱氢N-甲基化的关键。本文通过浸渍法制备了Cu/γ-Al_(2)O_(3)催化剂,在自制的连续流装置中,以苯胺合成N,N-二甲基苯胺为探针反应,系统考察了工艺条件对反应体系的影响,包括Cu负载量、反应温度、反应压力、反应空速。确定了最佳工艺条件,研究了该条件下该催化体系的稳定性,并进行了底物拓展。同时也对溶剂进行了拓展,以期为其他N-烷基化方法提供参考。Methanol as a carbon source is viewed as an effective and environmentally friendly method for in-situ liquid phase N-methylation of amine-based compounds.The development of efficient non-precious metal catalysts is the key to solve the N-methylation of methanol dehydrogenation.In this paper,Cu/γ-Al_(2)O_(3) catalyst was prepared by impregnation method.Using the synthesis of N,N-dimethylaniline from aniline as probe reaction,the influence of process conditions on the reaction system,including Cu load,reaction temperature,reaction pressure and reaction space velocity,was investigated systematically in a self-made continuous flow device.The optimum process conditions were determined,the stability of the catalytic system under these conditions was studied,and the substrate expansion was carried out.At the same time,the solvent was also expanded to provide reference for other N-alkylation methods.

关 键 词：胺类化合物 甲醇 N-甲基化 Cu/γ-Al_(2)O_(3) 连续流 反应工艺 

分 类 号：O621.251[理学—有机化学]