文章摘要
闫金辉,易颜辉,王丽,张睿,郭洪臣.铬催化剂促进CH4/NH3等离子体C-N偶联反应合成HCN[J].,2018,58(5):448-455
铬催化剂促进CH4/NH3等离子体C-N偶联反应合成HCN
Chromium catalyst promoted C-N coupling reaction in CH4/NH3 plasma for synthesis of hydrogen cyanide
  
DOI:10.7511/dllgxb201805002
中文关键词: 介质阻挡放电等离子体  催化  甲烷  氨气  氰化氢
英文关键词: dielectric barrier discharge plasma  catalysis  methane  ammonia  hydrogen cyanide
基金项目:国家自然科学基金资助项目(21503032);中国博士后科学基金资助项目(2015M5802202016T90217).
作者单位
闫金辉,易颜辉,王丽,张睿,郭洪臣  
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中文摘要:
      氰化氢作为一种重要的基本化工原料,在合成医药和精细化学品等领域有广泛用途.为解决氰化氢生产技术多在1 000 ℃以上的高温进行,且使用贵金属Pt或Pt-Rh催化剂的问题,在介质阻挡放电等离子体和负载型Cr催化剂条件下,通过CH4/NH3偶联反应一步合成氰化氢和乙腈等高附加值化合物,并系统研究了负载型Cr催化剂的负载量和载体类型对甲烷转化率和产物选择性的影响.在最优条件下(20 mL·min-1甲烷、40 mL·min-1氨气、负载量10%Cr/S-1催化剂、380 ℃反应温度),甲烷转化率达到30%左右,氰化氢选择性达到80%左右.该等离子体催化CH4/NH3偶联反应为氰化氢和乙腈提供了一种绿色且廉价的合成方法,也为甲烷和氨气精细化利用开辟了新途径.
英文摘要:
      Hydrogen cyanide, an important basic chemical stock, has been widely used in the synthesis of medicine and fine chemicals. However, hydrogen cyanide is usually produced at more than 1 000 ℃, in which, the noble metal catalysts, i. e., Pt or Pt-Rh alloy catalysts are employed necessarily. To solve this problem, using a dielectric barrier discharge plasma, CH4/NH3 coupling reaction can be promoted by Cr catalyst to synthesize hydrogen cyanide, with a by-product of acetonitrile. The effects of Cr loading and the support materials on the methane conversion and products selectivity are investigated. Under the optimized conditions (20 mL·min-1 CH4, 40 mL·min-1 NH3, 10% Cr/S-1 catalyst, 380 ℃), 30% methane conversion is obtained, along with 80% hydrogen cyanide selectivity. These experimental results indicate that the plasma-catalytic CH4/NH3 coupling reaction is a potential technology to provide a green and cheap method for the synthesis of hydrogen cyanide and acetonitrile, and to open a new way for fine application of CH4 and NH3.
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