SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2018, Vol. 26 ›› Issue (5): 1051-1058.DOI: 10.1016/j.cjche.2018.02.015

• Catalysis, Kinetics and Reaction Engineering • 上一篇    下一篇

Effect of copper precursors on the catalytic performance of Cu-ZSM-5 catalysts in N2O decomposition

Tao Meng1,2, Nan Ren3, Zhen Ma2,4   

  1. 1 School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 201418, China;
    2 Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, China;
    3 Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China;
    4 Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
  • 收稿日期:2017-08-05 修回日期:2018-01-16 出版日期:2018-05-28 发布日期:2018-06-29
  • 通讯作者: Nan Ren,E-mail addresses:nanren@fudan.edu.cn;Zhen Ma,E-mail addresses:zhenma@fudan.edu.cn
  • 基金资助:

    Supported by the National Natural Science Foundation of China (Grant No. 21477022).

Effect of copper precursors on the catalytic performance of Cu-ZSM-5 catalysts in N2O decomposition

Tao Meng1,2, Nan Ren3, Zhen Ma2,4   

  1. 1 School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 201418, China;
    2 Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai 200433, China;
    3 Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China;
    4 Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
  • Received:2017-08-05 Revised:2018-01-16 Online:2018-05-28 Published:2018-06-29
  • Contact: Nan Ren,E-mail addresses:nanren@fudan.edu.cn;Zhen Ma,E-mail addresses:zhenma@fudan.edu.cn
  • Supported by:

    Supported by the National Natural Science Foundation of China (Grant No. 21477022).

摘要: Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio=15) with aqueous solutions of different Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (Ⅱ) complex ion). After being pretreated in flowing He at 500℃ to form active Cu+, these catalysts exhibited quite different activities in catalytic decomposition of N2O. CZM-AC(Ⅱ) (prepared by ammoniacal copper (Ⅱ) complex ion) with 9.4 wt% Cu content was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2O conversion at 400℃. CZM-CA (prepared using Cu(CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2O conversion at 425℃. CZM-CC, CZMCN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(Ⅱ) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.

关键词: Copper precursor, Cu-ZSM-5, N2O decomposition, Catalysis, Catalyst, Zeolite

Abstract: Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio=15) with aqueous solutions of different Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (Ⅱ) complex ion). After being pretreated in flowing He at 500℃ to form active Cu+, these catalysts exhibited quite different activities in catalytic decomposition of N2O. CZM-AC(Ⅱ) (prepared by ammoniacal copper (Ⅱ) complex ion) with 9.4 wt% Cu content was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2O conversion at 400℃. CZM-CA (prepared using Cu(CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2O conversion at 425℃. CZM-CC, CZMCN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(Ⅱ) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.

Key words: Copper precursor, Cu-ZSM-5, N2O decomposition, Catalysis, Catalyst, Zeolite