Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

doi:10.1016/j.cjche.2024.03.022

中国化学工程学报 ›› 2024, Vol. 71 ›› Issue (7): 172-182.DOI: 10.1016/j.cjche.2024.03.022

Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

Runnong Yang^1,2,5, Wuyuan Liu², Zhaoying Wang², Ming Sun^1,2, Guangying Fu³, Zihan Gao², Wenjian Jiao⁴, Rui Li³, Lin Yu^1,2

1. Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, China;
2. Guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China;
3. Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China;
4. Testing and Certification Business Department, China Automotive Technology and Research Center Company Limited, Wuhan 430056, China;
5. Guangdong Foran Technology Company Limited, Foshan 528000, China

收稿日期:2023-09-11 修回日期:2024-03-11 出版日期:2024-07-28 发布日期:2024-08-30
通讯作者: Lin Yu,E-mail:gych@gdut.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (22278086). Thanks to the technique support of the Analysis and Test Center of the Guangdong University of Technology.

Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

Runnong Yang^1,2,5, Wuyuan Liu², Zhaoying Wang², Ming Sun^1,2, Guangying Fu³, Zihan Gao², Wenjian Jiao⁴, Rui Li³, Lin Yu^1,2

1. Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, China;
2. Guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China;
3. Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China;
4. Testing and Certification Business Department, China Automotive Technology and Research Center Company Limited, Wuhan 430056, China;
5. Guangdong Foran Technology Company Limited, Foshan 528000, China

Received:2023-09-11 Revised:2024-03-11 Online:2024-07-28 Published:2024-08-30
Contact: Lin Yu,E-mail:gych@gdut.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (22278086). Thanks to the technique support of the Analysis and Test Center of the Guangdong University of Technology.

摘要/Abstract

摘要： The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH₃ (NH₃-SCR). In order to further improve the catalytic property, a series of Mn ion-assisted Cu/SSZ-13 powder catalysts were prepared by co-exchange method and stepwise exchange method. It is found that the NH₃-SCR activity, N₂ selectivity, hydrothermal stability and sulfur resistance of Cu/SSZ-13 are promoted by introducing a minority of Mn (0.15% to 0.23% (mass)) through co-exchange method. Characterization results reveal that the Cu, Mn co-exchange enables the higher amounts of Cu²⁺ active sites, the abundant medium strong and strong acid, the optimized ratio of Lewis acid to Brønsted acid etc., which are required for a good NH₃-SCR catalytic property over broad temperature range and under harsh working environment. Moreover, a monolithic catalyst was prepared by impregnating a cordierite ceramic support into the coating slurry containing the optimized CuMn/SSZ-13 powder. The diesel engine bench tests show that Cu, Mn co-exchange gives the monolith catalyst a better catalytic property than commercial catalysts. This work provides an important guidance for the rational design of secondary-ion-assisted zeolites applied in NH₃-SCR.

关键词: MnCu/SSZ-13, Co-exchange, Zeolite, Catalysis, Selective catalytic reduction

Abstract: The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH₃ (NH₃-SCR). In order to further improve the catalytic property, a series of Mn ion-assisted Cu/SSZ-13 powder catalysts were prepared by co-exchange method and stepwise exchange method. It is found that the NH₃-SCR activity, N₂ selectivity, hydrothermal stability and sulfur resistance of Cu/SSZ-13 are promoted by introducing a minority of Mn (0.15% to 0.23% (mass)) through co-exchange method. Characterization results reveal that the Cu, Mn co-exchange enables the higher amounts of Cu²⁺ active sites, the abundant medium strong and strong acid, the optimized ratio of Lewis acid to Brønsted acid etc., which are required for a good NH₃-SCR catalytic property over broad temperature range and under harsh working environment. Moreover, a monolithic catalyst was prepared by impregnating a cordierite ceramic support into the coating slurry containing the optimized CuMn/SSZ-13 powder. The diesel engine bench tests show that Cu, Mn co-exchange gives the monolith catalyst a better catalytic property than commercial catalysts. This work provides an important guidance for the rational design of secondary-ion-assisted zeolites applied in NH₃-SCR.

Key words: MnCu/SSZ-13, Co-exchange, Zeolite, Catalysis, Selective catalytic reduction

Runnong Yang, Wuyuan Liu, Zhaoying Wang, Ming Sun, Guangying Fu, Zihan Gao, Wenjian Jiao, Rui Li, Lin Yu. Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust[J]. 中国化学工程学报, 2024, 71(7): 172-182.

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Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

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