能源化学(英文) ›› 2015, Vol. 21 ›› Issue (2): 219-224.DOI: 10.1016/S2095-4956(15)60304-7

• ARTICLES • 上一篇    下一篇

Identification of the starting reaction position in the hydrogenation of (N-ethyl)carbazole over Raney-Ni

Feifei Sun, Yue An, Lecheng Lei, Fuying Wu, Jingke Zhu, Xingwang Zhang   

  1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemical and Biological Engineering,Zhejiang University, Hangzhou 310027, Zhejiang, China
  • 收稿日期:2014-09-12 修回日期:2014-11-14 出版日期:2015-03-23 发布日期:2015-03-23
  • 通讯作者: Xingwang Zhang
  • 基金资助:

    This work was supported by the National Natural Science Foundation of China (U1162127, U1462201, 21076189, 21476202 and 21276231).

Identification of the starting reaction position in the hydrogenation of (N-ethyl)carbazole over Raney-Ni

Feifei Sun, Yue An, Lecheng Lei, Fuying Wu, Jingke Zhu, Xingwang Zhang   

  1. Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Department of Chemical and Biological Engineering,Zhejiang University, Hangzhou 310027, Zhejiang, China
  • Received:2014-09-12 Revised:2014-11-14 Online:2015-03-23 Published:2015-03-23
  • Contact: Xingwang Zhang
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (U1162127, U1462201, 21076189, 21476202 and 21276231).

摘要: Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rate-limiting step during the period, in which the conversion of carbazole was less than 40%. The hydrogenation process followed pseudo-first-order kinetics and the hydrogenation activation energies of carbazole and N-ethylcarbazole were 90kJ/mol and 115kJ/mol, respectively. The reaction starting position as well as the pathway of the hydrogenation of (N-ethyl)carbazole were investigated by comparing the kinetic characteristics of hydrogen uptake of carbazole and N-ethylcarbazole. The results showed that the reaction was a stepwise hydrogenation process and the first H2 was added to the C1=C10 double bond in the hydrogenation.

关键词: (N-ethyl)carbazole, hydrogen storage, Raney-Ni catalyst, reaction kinetics, first reaction position

Abstract: Hydrogenation of carbazole and N-ethylcarbazole over Raney-Ni catalyst were realized in the temperature range of 393-503K. 4[H] adduct dominated the hydrogenation products and the formation of 2[H] adduct was the rate-limiting step during the period, in which the conversion of carbazole was less than 40%. The hydrogenation process followed pseudo-first-order kinetics and the hydrogenation activation energies of carbazole and N-ethylcarbazole were 90kJ/mol and 115kJ/mol, respectively. The reaction starting position as well as the pathway of the hydrogenation of (N-ethyl)carbazole were investigated by comparing the kinetic characteristics of hydrogen uptake of carbazole and N-ethylcarbazole. The results showed that the reaction was a stepwise hydrogenation process and the first H2 was added to the C1=C10 double bond in the hydrogenation.

Key words: (N-ethyl)carbazole, hydrogen storage, Raney-Ni catalyst, reaction kinetics, first reaction position