SCI和EI收录∣中国化工学会会刊

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 Qiu1,2, Yonghou Xiao1,2, Haoran Wu2, Shengnan Lu3, Qidong Zhao2, Gaohong He1,2   

  1. 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 Qiu1,2, Yonghou Xiao1,2, Haoran Wu2, Shengnan Lu3, Qidong Zhao2, Gaohong He1,2   

  1. 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: 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 NOx conversion of 99% was attained; the NOx 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 DeNOx, 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 NOx conversion of 99% was attained; the NOx 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 DeNOx, One-pot synthesis