SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2014, Vol. 22 ›› Issue (5): 607-610.DOI: 10.1016/S1004-9541(14)60097-5

• 催化、动力学与反应工程 • 上一篇    

Influence of Solvent on Reaction Path to Synthesis of Methyl N-Phenyl Carbamate from Aniline, CO2 and Methanol

安华良, 张丽丽, 苑保国, 赵新强, 王延吉   

  1. Hebei Provincial Key Lab of Green Chemical Technology and Efficient Energy Saving, Hebei University of Technology, Tianjin 300130, China
  • 收稿日期:2013-09-29 修回日期:2013-12-31 出版日期:2014-05-28 发布日期:2014-05-06
  • 通讯作者: ZHAO Xinqiang,E-mail: zhaoxq@hebut.edu.cn
  • 基金资助:

    Supported by the National Natural Science Foundation of China (20976035), the Natural Science Foundation of Tianjin City (12JCYBJC12800) and the Key Basic Research Project of Applied Basic Research Plan of Hebei Province (12965642D).

Influence of Solvent on Reaction Path to Synthesis of Methyl N-Phenyl Carbamate from Aniline, CO2 and Methanol

AN Hualiang, ZHANG Lili, YUAN Baoguo, ZHAO Xinqiang, WANG Yanji   

  1. Hebei Provincial Key Lab of Green Chemical Technology and Efficient Energy Saving, Hebei University of Technology, Tianjin 300130, China
  • Received:2013-09-29 Revised:2013-12-31 Online:2014-05-28 Published:2014-05-06
  • Supported by:

    Supported by the National Natural Science Foundation of China (20976035), the Natural Science Foundation of Tianjin City (12JCYBJC12800) and the Key Basic Research Project of Applied Basic Research Plan of Hebei Province (12965642D).

摘要: Methyl N-phenyl carbamate (MPC), an important organic chemical, can be synthesized from aniline, CO2 and methanol. Catalyst Cu-Fe/ZrO2-SiO2 was first prepared and its catalytic performance for MPC synthesis was evaluated. Then the influence of solvent on the reaction path of MPC synthesis was investigated. It is found that the reaction intermediate is different with acetonitrile or methanol as a solvent. With acetonitrile as a solvent, the synthesis of MPC follows the reaction path with diphenyl urea as the intermediate, while with methanol as a solvent the reaction occurs via the reaction path with dimethyl carbonate as the intermediate. The catalytic mechanism of cooperative catalysis comprising metal sites, Lewis acid sites and Lewis base sites is proposed according to different reaction intermediates.

关键词: reaction path, methyl N-phenyl carbamate, CO2, aniline, methanol, Cu-Fe/ZrO2-SiO2 catalyst

Abstract: Methyl N-phenyl carbamate (MPC), an important organic chemical, can be synthesized from aniline, CO2 and methanol. Catalyst Cu-Fe/ZrO2-SiO2 was first prepared and its catalytic performance for MPC synthesis was evaluated. Then the influence of solvent on the reaction path of MPC synthesis was investigated. It is found that the reaction intermediate is different with acetonitrile or methanol as a solvent. With acetonitrile as a solvent, the synthesis of MPC follows the reaction path with diphenyl urea as the intermediate, while with methanol as a solvent the reaction occurs via the reaction path with dimethyl carbonate as the intermediate. The catalytic mechanism of cooperative catalysis comprising metal sites, Lewis acid sites and Lewis base sites is proposed according to different reaction intermediates.

Key words: reaction path, methyl N-phenyl carbamate, CO2, aniline, methanol, Cu-Fe/ZrO2-SiO2 catalyst