SCI和EI收录∣中国化工学会会刊

›› 2015, Vol. 23 ›› Issue (2): 446-450.DOI: 10.1016/j.cjche.2014.03.002

• 研究简报 • 上一篇    下一篇

Heterogeneous synthesis of dimethylhexane-1,6-dicarbamate from 1,6-hexanediamine and methyl carbonate in methanol over a CeO2 catalyst

Yan Cao, Huiquan Li, Xintao Li, Liguo Wang, Ganyu Zhu, Qing Tang   

  1. Key Laboratory of Green Process and Engineering, National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Sciences(CAS), Beijing 100190, China
  • 收稿日期:2013-11-01 修回日期:2014-03-12 出版日期:2015-02-28 发布日期:2015-03-01
  • 通讯作者: Huiquan Li
  • 基金资助:
    Supported by the Science and Technology Ministry of China (2013BAC11B03) and National Nature Science Foundation of China (21476244, 21206180, 21406245).

Heterogeneous synthesis of dimethylhexane-1,6-dicarbamate from 1,6-hexanediamine and methyl carbonate in methanol over a CeO2 catalyst

Yan Cao, Huiquan Li, Xintao Li, Liguo Wang, Ganyu Zhu, Qing Tang   

  1. Key Laboratory of Green Process and Engineering, National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Sciences(CAS), Beijing 100190, China
  • Received:2013-11-01 Revised:2014-03-12 Online:2015-02-28 Published:2015-03-01
  • Supported by:
    Supported by the Science and Technology Ministry of China (2013BAC11B03) and National Nature Science Foundation of China (21476244, 21206180, 21406245).

摘要: The efficient synthesis of dimethylhexane-1,6-dicarbamate (HDC) from 1,6-hexanediamine (HDA) and methyl carbonate over a series of heterogeneous catalysts (e.g., MgO, Fe2O3, Mo2O3, and CeO2) was investigated. The reaction pathway was confirmed as an alcoholysis reaction through a series of designed experiments. Under optimized conditions, 100% HDA conversion with 83.1% HDCtotal and 16.9% polyurea was obtained using a onestep with high temperature procedurewith CeO2 as the catalyst. A newtwo-stepwith variable temperature technology was developed based on the reaction pathway to reduce the polyurea yield. Using the proposed method, the HDCtotal yield reached 95.2%, whereas the polyurea yield decreased to 4.8%. The CeO2 catalyst showed high stability and did not exhibit any observable decrease in the HDC yield or any structural changes after four recycling periods.

关键词: Heterogeneous, Dimethylhexane-1,6-dicarbamate, Methyl carbonate, Reaction pathway, Two-step variable-temperature technology

Abstract: The efficient synthesis of dimethylhexane-1,6-dicarbamate (HDC) from 1,6-hexanediamine (HDA) and methyl carbonate over a series of heterogeneous catalysts (e.g., MgO, Fe2O3, Mo2O3, and CeO2) was investigated. The reaction pathway was confirmed as an alcoholysis reaction through a series of designed experiments. Under optimized conditions, 100% HDA conversion with 83.1% HDCtotal and 16.9% polyurea was obtained using a onestep with high temperature procedurewith CeO2 as the catalyst. A newtwo-stepwith variable temperature technology was developed based on the reaction pathway to reduce the polyurea yield. Using the proposed method, the HDCtotal yield reached 95.2%, whereas the polyurea yield decreased to 4.8%. The CeO2 catalyst showed high stability and did not exhibit any observable decrease in the HDC yield or any structural changes after four recycling periods.

Key words: Heterogeneous, Dimethylhexane-1,6-dicarbamate, Methyl carbonate, Reaction pathway, Two-step variable-temperature technology