One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH3 at low temperature

doi:10.1016/j.cjche.2022.07.020

中国化学工程学报 ›› 2023, Vol. 56 ›› Issue (4): 193-202.DOI: 10.1016/j.cjche.2022.07.020

• Full Length Article • 上一篇下一篇

One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH₃ at low temperature

Shuang Qiu^1,2, Yonghou Xiao^1,2, Haoran Wu², Shengnan Lu³, Qidong Zhao², Gaohong He^1,2

1. Panjin Institute of Industrial Technology, Liaoning Key Laboratory of Chemical Additive Synthesis and Separation, Dalian University of Technology, Panjin 124221, China;
2. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Panjin 124221, China;
3. School of Petrochemical Engineering, Shenyang University of Technology, Liaoyang 111003, China

收稿日期:2022-05-04 修回日期:2022-06-28 出版日期:2023-04-28 发布日期:2023-06-13
通讯作者: Yonghou Xiao,E-mail:yonghou.xiao@dlut.edu.cn
基金资助:
This research was supported by Project of Central Government for Local Science and Technology Development of China (2022JH6/100100050), the National Natural Science Foundation of China (21776028), and Liaoning Key Laboratory of Chemical Additive Synthesis and Separation (ZJKF2001).

One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH₃ at low temperature

Shuang Qiu^1,2, Yonghou Xiao^1,2, Haoran Wu², Shengnan Lu³, Qidong Zhao², Gaohong He^1,2

1. Panjin Institute of Industrial Technology, Liaoning Key Laboratory of Chemical Additive Synthesis and Separation, Dalian University of Technology, Panjin 124221, China;
2. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Panjin 124221, China;
3. School of Petrochemical Engineering, Shenyang University of Technology, Liaoyang 111003, China

Received:2022-05-04 Revised:2022-06-28 Online:2023-04-28 Published:2023-06-13
Contact: Yonghou Xiao,E-mail:yonghou.xiao@dlut.edu.cn
Supported by:
This research was supported by Project of Central Government for Local Science and Technology Development of China (2022JH6/100100050), the National Natural Science Foundation of China (21776028), and Liaoning Key Laboratory of Chemical Additive Synthesis and Separation (ZJKF2001).

摘要/Abstract

摘要： NH₃ selective catalytic reduction (SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The CeCu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02% (mass) Ce constituent exhibited the best catalytic activity below 300 ℃ and a maximum NO_x conversion of 99% was attained; the NO_x removal rates of more than 68% and 94% were achieved at 150 ℃ and 200 ℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH₃-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Brønsted acid centers and promote the synergistic effect between CuO grains and isolated Cu²⁺ to enhance the redox cycle, which benefit the NH₃-SCR reaction. This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature.

关键词: CeCu-SAPO-34, Selective catalytic reduction (SCR), Low temperature DeNO_x, One-pot synthesis

Abstract: NH₃ selective catalytic reduction (SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The CeCu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02% (mass) Ce constituent exhibited the best catalytic activity below 300 ℃ and a maximum NO_x conversion of 99% was attained; the NO_x removal rates of more than 68% and 94% were achieved at 150 ℃ and 200 ℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH₃-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Brønsted acid centers and promote the synergistic effect between CuO grains and isolated Cu²⁺ to enhance the redox cycle, which benefit the NH₃-SCR reaction. This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature.

Key words: CeCu-SAPO-34, Selective catalytic reduction (SCR), Low temperature DeNO_x, One-pot synthesis

Shuang Qiu, Yonghou Xiao, Haoran Wu, Shengnan Lu, Qidong Zhao, Gaohong He. One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH₃ at low temperature[J]. 中国化学工程学报, 2023, 56(4): 193-202.

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One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH₃ at low temperature

One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH₃ at low temperature

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