Acta Phys. -Chim. Sin. ›› 2018, Vol. 34 ›› Issue (3): 247-255.doi: 10.3866/PKU.WHXB201708171

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Plasma-Triggered CH3OH/NH3 Coupling Reaction for Synthesis of Nitrile Compounds

Yanhui YI1,*(),Xunxun WANG1,Li WANG1,Jinhui YAN1,Jialiang ZHANG2,Hongchen GUO1,*()   

  1. 1 State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
    2 School of Physics and Optoelectronic Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China
  • Received:2017-06-22 Published:2017-12-18
  • Contact: Yanhui YI,Hongchen GUO E-mail:yiyanhui@dlut.edu.cn;hongchenguo@163.com
  • Supported by:
    The project was supported by the Natural Science Foundation of China(21503032);China Postdoctoral Science Foundation(2015M580220);China Postdoctoral Science Foundation(2016T90217)

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.

Key words: DBD plasma, Methanol, Ammonia, Coupling reaction, Nitrile compounds

MSC2000: 

  • O644.29