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发表时间：2022-10-06

发表刊物：物理化学学报

所属单位：化工学院

卷号：34

期号：3

页面范围：247-255

ISSN号：1000-6818

摘要：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 CH_3OH/NH_3 coupling reaction can directly
   synthesize N,N-dimethyl cyanamide[(CH_3)_2NCN],amino acetonitrile
   [NH_2CH_2CN], and N,N-dimethyl amino acetonitrile [(CH_3)_2NCH_2CN],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 CH_3OH/NH_3
   plasma could be a key reactive intermediate aiding in the synthesis of
   nitrile compounds. The CH_3OH/NH_3 plasma coupling reaction process is
   an environment-friendly methodology for the synthesis of (CH_3)_2NCN,
   NH_2CH_2CN, and (CH_3)_2NCH_2CN,and is a potential novel pathway for the
   synthesis of fine chemicals like methanol and ammonia.

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