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

doi:10.1016/j.cjche.2021.06.012

Chinese Journal of Chemical Engineering ›› 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 NO_x by NH₃

Xin Yong², Hong Chen¹, Huawang Zhao², Miao Wei², Yingnan Zhao³, Yongdan Li^2,3

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:2022-07-20 Published:2022-06-28
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.

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

Xin Yong², Hong Chen¹, Huawang Zhao², Miao Wei², Yingnan Zhao³, Yongdan Li^2,3

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

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.

Abstract

Abstract: The effects of SO₂ on an one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NO_x by NH₃ were examined. The addition of SO₂ inhibited NO_x conversion significantly below 300 ℃, while no effect on NO_x 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 deNO_x 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

摘要： The effects of SO₂ on an one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NO_x by NH₃ were examined. The addition of SO₂ inhibited NO_x conversion significantly below 300 ℃, while no effect on NO_x 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 deNO_x 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

Xin Yong, Hong Chen, Huawang Zhao, Miao Wei, Yingnan Zhao, Yongdan Li. Insight into SO₂ poisoning and regeneration of one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NO_x by NH₃[J]. Chinese Journal of Chemical Engineering, 2022, 46(6): 184-193.

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

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

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