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

doi:10.1016/j.cjche.2018.02.015

Chin.J.Chem.Eng. ›› 2018, Vol. 26 ›› Issue (5): 1051-1058.DOI: 10.1016/j.cjche.2018.02.015

• Catalysis, kinetics and reaction engineering • Previous Articles Next Articles

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

Tao Meng^1,2, Nan Ren³, Zhen Ma^2,4

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:2018-06-29 Published:2018-05-28
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).

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

Tao Meng^1,2, Nan Ren³, Zhen Ma^2,4

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

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).

Abstract

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

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

Tao Meng, Nan Ren, Zhen Ma. Effect of copper precursors on the catalytic performance of Cu-ZSM-5 catalysts in N₂O decomposition[J]. Chin.J.Chem.Eng., 2018, 26(5): 1051-1058.

Tao Meng, Nan Ren, Zhen Ma. Effect of copper precursors on the catalytic performance of Cu-ZSM-5 catalysts in N₂O decomposition[J]. Chinese Journal of Chemical Engineering, 2018, 26(5): 1051-1058.

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

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

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