The Catalytic Pathways of Hydrohalogenation over Metal-Free Nitrogen-Doped Carbon Nanotubes

Authors

  • Kai Zhou,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Dr. Bo Li,

    1. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, 110016 Shenyang (PR China)
    Search for more papers by this author
  • Prof. Qiang Zhang,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Dr. Jia-Qi Huang,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Gui-Li Tian,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Jin-Chao Jia,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Dr. Meng-Qiang Zhao,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Prof. Guo-Hua Luo,

    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    Search for more papers by this author
  • Prof. Dang Sheng Su,

    Corresponding author
    1. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, 110016 Shenyang (PR China)
    2. Department of Inorganic Chemistry, Fritz Haber Institute of the Max Plank Society, Faradayweg 4–6, 14195 Berlin (Germany)
    • Dang Sheng Su, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, 110016 Shenyang (PR China)

      Fei Wei, Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051

    Search for more papers by this author
  • Prof. Fei Wei

    Corresponding author
    1. Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051
    • Dang Sheng Su, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, 110016 Shenyang (PR China)

      Fei Wei, Beijing Key Laboratory of Green Chemical Reaction, Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084 Beijing (PR China), Fax: (+86) 10-6277-2051

    Search for more papers by this author

Abstract

Nitrogen-doped carbon nanotubes (N-CNTs) are found to be active as one novel heterogeneous catalyst for acetylene hydrochlorination reaction, possessing good activity (TOF=2.3×10−3 s−1) and high selectivity (>98 %). Compared to toxic and energy-consuming conventional catalysts, such as HgCl2, N-CNTs are more favorable in terms of sustainability, because of their thermo-stability, metal-free make up, and the wide availability of bulk CNT. Coupling X-ray photoelectron spectroscopy and density functional theory computations (DFT), the main active source and reaction pathway are shown. Good linearity between the quaternary nitrogen content and conversion is revealed. DFT study shows that the nitrogen doping enhanced the formation of the covalent bond between C2H2 and NCNT compared with the undoped CNT, and therefore promoted the addition reaction of the C2H2 and HCl into C2H3Cl.

Ancillary