Acta Phys. -Chim. Sin. ›› 2015, Vol. 31 ›› Issue (5): 941-947.doi: 10.3866/PKU.WHXB201503051

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Influence of Oxidation State of Nickel Supported on TiO2 on Gas-Phase Hydrogenation of Acetonitrile

XIA Long-Fei1, JIANG Zhi1, SHANGGUAN Wen-Feng1, GU Shun-Chao2,3, HIRANO Shinichi3   

  1. 1 School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China;
    2 School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China;
    3 Hirano Institute for Materials Innovation, Shanghai Jiao Tong University, Shanghai 200240, P. R. China
  • Received:2014-12-09 Revised:2015-02-09 Published:2015-05-08
  • Contact: SHANGGUAN Wen-Feng E-mail:shangguan@sjtu.edu.cn
  • Supported by:

    The project was supported by the Project of Kao Corporation (Japan).

Abstract:

Nickel catalysts supported on TiO2 were prepared using an impregnation method. Changes in the reduction temperature from 200 to 400 ℃ resulted in dispersion of nickel with different oxidation states on TiO2. The gas-phase hydrogenation of acetonitrile was found to be influenced by the nickel oxidation state. Nickel reduced at 300 ℃ gave the highest acetonitrile conversion ratio, i.e., about 100%, when the reaction temperature was 100 ℃. The product yields depend on the amount of acidic sites on Ni/TiO2 catalysts; this can be influenced not only by the TiO2 support, but also by the properties of the supported nickel nanoparticles. The triethylamine yield increased to a maximum (from 34% to about 48%) with increasing reduction temperature; this corresponded to the gradual appearance of Ni0 in Ni/TiO2 and a decrease in the intrinsic acidity of the Ni/TiO2 catalyst. Triethylamine was the initial product in the hydrogenation of acetonitrile with Ni/TiO2. The oxidation state of nickel influenced not only the conversion of acetonitrile but also desorption of the final products. Amechanism for the first step in this reaction is proposed.

Key words: Gas-phase hydrogenation of acetonitrile, Impregnation method, TiO2, Ni, Amine

MSC2000: 

  • O643