| 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 |
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| 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). |
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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CH4/NH3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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