物理化学学报2018，Vol.34Issue(3)：247-255,9.DOI:10.3866/PKU.WHXB201708171
等离子体引发CH3OH/NH3偶联反应合成腈类化合物
Plasma-Triggered CH3OH/NH3 Coupling Reaction for Synthesis of Nitrile Compounds
摘要
Abstract
Nitriles are very important for the synthesis of fine chemicals and medicines.However,many nitriles are not widely available,as their synthesis processes pose a serious risk to the environment.Herein,we report that a spontaneous CH3OH/NH3 coupling reaction can directly synthesize N,N-dimethyl cyanamide[(CH3)2NCN],amino acetonitrile [NH2CH2CN],and N,N-dimethyl amino acetonitrile [(CH3)2NCH2CN],when a mixture of methanol and ammonia is transferred into the plasma state via a dielectric barrier discharge.The effects of the plasma reactor configuration,discharge conditions,reaction conditions,and packing materials on the methanol conversion as well as the product selectivity were systematically investigated.Experimental results indicate that,under optimized conditions,a nitrile compound selectivity of 22.1％ with a methanol conversion of 51.5％ could be achieved.Analysis by optical emission spectroscopy indicates that the C=N species in CH3OH/NH3 plasma could be a key reactive intermediate aiding in the synthesis of nitrile compounds.The CH3OH/NH3 plasma coupling reaction process is an environment-friendly methodology for the synthesis of (CH3)2NCN,NH2CH2CN,and (CH3)2NCH2CN,and is a potential novel pathway for the synthesis of fine chemicals like methanol and ammonia.关键词
介质阻挡放电等离子体/甲醇/氨气/偶联反应/腈类化合物Key words
DBD plasma/Methanol/Ammonia/Coupling reaction/Nitrile compounds分类
化学化工引用本文复制引用
易颜辉,王旬旬,王丽,闫金辉,张家良,郭洪臣..等离子体引发CH3OH/NH3偶联反应合成腈类化合物[J].物理化学学报,2018,34(3):247-255,9.基金项目
The project was supported by the Natural Science Foundation of China (21503032) and China Postdoctoral Science Foundation (2015M580220,2016T90217).国家自然科学基金(21503032)和中国博士后科学基金(2015M580220,2016T90217)资助 （21503032）
