SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 46 ›› Issue (6): 184-193.DOI: 10.1016/j.cjche.2021.06.012

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Insight into SO2 poisoning and regeneration of one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NOx by NH3

Xin Yong2, Hong Chen1, Huawang Zhao2, Miao Wei2, Yingnan Zhao3, Yongdan Li2,3   

  1. 1 School of Environmental Engineering, Tianjin University, Tianjin 300072, China;
    2 Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Technology, State Key Laboratory of Chemical Engineering (Tianjin University), School of Chemical Engineering, Tianjin University, Tianjin 300072, China;
    3 Department of Chemical and Metallurgical Engineering, School of Chemical Engineering, Aalto University, Espoo 02150, Finland
  • 收稿日期:2021-03-28 修回日期:2021-06-07 出版日期:2022-06-28 发布日期:2022-07-20
  • 通讯作者: Hong Chen,E-mail:chenhong_0405@tju.edu.cn;Yongdan Li,E-mail:yongdan.li@aalto.fi
  • 基金资助:
    Financial supports from the Natural Science Foundation of Tianjin 19JCTPJC42300.

Insight into SO2 poisoning and regeneration of one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NOx by NH3

Xin Yong2, Hong Chen1, Huawang Zhao2, Miao Wei2, Yingnan Zhao3, Yongdan Li2,3   

  1. 1 School of Environmental Engineering, Tianjin University, Tianjin 300072, China;
    2 Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Technology, State Key Laboratory of Chemical Engineering (Tianjin University), School of Chemical Engineering, Tianjin University, Tianjin 300072, China;
    3 Department of Chemical and Metallurgical Engineering, School of Chemical Engineering, Aalto University, Espoo 02150, Finland
  • Received:2021-03-28 Revised:2021-06-07 Online:2022-06-28 Published:2022-07-20
  • Contact: Hong Chen,E-mail:chenhong_0405@tju.edu.cn;Yongdan Li,E-mail:yongdan.li@aalto.fi
  • Supported by:
    Financial supports from the Natural Science Foundation of Tianjin 19JCTPJC42300.

摘要: The effects of SO2 on an one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NOx by NH3 were examined. The addition of SO2 inhibited NOx conversion significantly below 300 ℃, while no effect on NOx conversion was observed above 300 ℃. TGA, TPD, and XPS results showed that the deactivation was caused by the formation of (NH4)2SO4, SO2 chemisorption on the isolated Cu2+ ion sites, as well as the formation of CuSO4-like species. Among them, the site-blocking effect of (NH4)2SO4 on Cu2+ was the primary reason for deactivation. Fortunately, 89% of deNOx activity of the poisoned catalyst was recovered after thermal treatment at 500 ℃ in air, where (NH4)2SO4 was completely decomposed. The activity was further recovered with regeneration temperature increasing to 600 ℃, removing the adsorbed SO2 on the Cu2+ sites. The regeneration at 600 ℃ could not recover the activity completely, because of the high stability of CuSO4-like species.

关键词: Emission control, SCR, One-pot synthesis of Cu-SSZ-13, SO2 poisoning, Activity regeneration

Abstract: The effects of SO2 on an one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NOx by NH3 were examined. The addition of SO2 inhibited NOx conversion significantly below 300 ℃, while no effect on NOx conversion was observed above 300 ℃. TGA, TPD, and XPS results showed that the deactivation was caused by the formation of (NH4)2SO4, SO2 chemisorption on the isolated Cu2+ ion sites, as well as the formation of CuSO4-like species. Among them, the site-blocking effect of (NH4)2SO4 on Cu2+ was the primary reason for deactivation. Fortunately, 89% of deNOx activity of the poisoned catalyst was recovered after thermal treatment at 500 ℃ in air, where (NH4)2SO4 was completely decomposed. The activity was further recovered with regeneration temperature increasing to 600 ℃, removing the adsorbed SO2 on the Cu2+ sites. The regeneration at 600 ℃ could not recover the activity completely, because of the high stability of CuSO4-like species.

Key words: Emission control, SCR, One-pot synthesis of Cu-SSZ-13, SO2 poisoning, Activity regeneration