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Nano Research 2023, 16(10): 12126-12133 https://doi.org/10.1007/s12274-023-5500-x
Research Article | Issue | Published: 27 February 2023

La ions-enhanced NH3-SCR performance over Cu-SSZ-13 catalysts

Show Author's Information Mengyang Chen1,3,§,  Wenru Zhao2,§,  Yingzhen Wei1,  Jinfeng Han1,  Junyan Li1,  Chang Sun1,  Donghai Mei2( ),  Jihong Yu1,3( )
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
School of Materials Science and Engineering, Tiangong University, Tianjin 300387, China
International Center of Future Science, Jilin University, Changchun 130012, China

§ Mengyang Chen and Wenru Zhao contributed equally to this work.

Keywords:
zeolite, bimetallic catalyst, Cu-SSZ-13, lanthanum, ammonia selective catalytic reduction (NH3-SCR)
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Chen M, Zhao W, Wei Y, et al. La ions-enhanced NH3-SCR performance over Cu-SSZ-13 catalysts. Nano Research, 2023, 16(10): 12126-12133. https://doi.org/10.1007/s12274-023-5500-x
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Abstract Full text Electronic supplementary material About this article

Lanthanum (La) ions are generally recognized to cause a decline of the catalytic performance for Cu-SSZ-13 zeolite in the selective catalytic reduction of NOx with NH3 (NH3-SCR). Herein, we demonstrate that the NH3-SCR performance and hydrothermal stability of Cu-La-SSZ-13 zeolites can be enhanced with the incorporation of a small amount of La ions. The incorporation of La ions into SSZ-13 favors more Z2Cu2+ ions at six-membered rings (6MRs), which results in higher hydrothermal stability of Cu-La-SSZ-13 than that of Cu-SSZ-13. The NO conversion of Cu-La-SSZ-13 achieves 5%–10% higher than that of Cu-SSZ-13 at the temperature range of 400–550 °C after hydrothermal ageing. While introducing excess amount of La ions in SSZ-13 may cause the formation of inactive CuOx, leading to the decrease of catalytic activity and hydrothermal stability. Notably, the low-temperature activity of Cu-SSZ-13 with a low Cu content (≤ 2 wt.%) can be boosted by the introduction of La ions, which is largely due to the improved redox ability of Cu active sites modified by La ions. Density functional theory (DFT) calculations indicate that La ions prefer to locate at eight-membered rings (8MRs) and thus promoting the formation of more Z2Cu2+ ions. Meanwhile, the existence of La ions in SSZ-13 inhibits the dealumination process and the transformation from Z2Cu2+ to CuOx, resulting in its enhanced hydrothermal stability. The present work sheds a new insight into the regulation of secondary metal cations for promoting high NH3-SCR performance over Cu-SSZ-13 zeolite catalysts.


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About this article

La ions-enhanced NH3-SCR performance over Cu-SSZ-13 catalysts

Show Author's information Mengyang Chen1,3,§, Wenru Zhao2,§, Yingzhen Wei1, Jinfeng Han1, Junyan Li1, Chang Sun1, Donghai Mei2( ), Jihong Yu1,3( )
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
School of Materials Science and Engineering, Tiangong University, Tianjin 300387, China
International Center of Future Science, Jilin University, Changchun 130012, China

§ Mengyang Chen and Wenru Zhao contributed equally to this work.

Abstract

Lanthanum (La) ions are generally recognized to cause a decline of the catalytic performance for Cu-SSZ-13 zeolite in the selective catalytic reduction of NOx with NH3 (NH3-SCR). Herein, we demonstrate that the NH3-SCR performance and hydrothermal stability of Cu-La-SSZ-13 zeolites can be enhanced with the incorporation of a small amount of La ions. The incorporation of La ions into SSZ-13 favors more Z2Cu2+ ions at six-membered rings (6MRs), which results in higher hydrothermal stability of Cu-La-SSZ-13 than that of Cu-SSZ-13. The NO conversion of Cu-La-SSZ-13 achieves 5%–10% higher than that of Cu-SSZ-13 at the temperature range of 400–550 °C after hydrothermal ageing. While introducing excess amount of La ions in SSZ-13 may cause the formation of inactive CuOx, leading to the decrease of catalytic activity and hydrothermal stability. Notably, the low-temperature activity of Cu-SSZ-13 with a low Cu content (≤ 2 wt.%) can be boosted by the introduction of La ions, which is largely due to the improved redox ability of Cu active sites modified by La ions. Density functional theory (DFT) calculations indicate that La ions prefer to locate at eight-membered rings (8MRs) and thus promoting the formation of more Z2Cu2+ ions. Meanwhile, the existence of La ions in SSZ-13 inhibits the dealumination process and the transformation from Z2Cu2+ to CuOx, resulting in its enhanced hydrothermal stability. The present work sheds a new insight into the regulation of secondary metal cations for promoting high NH3-SCR performance over Cu-SSZ-13 zeolite catalysts.

Keywords: zeolite, bimetallic catalyst, Cu-SSZ-13, lanthanum, ammonia selective catalytic reduction (NH3-SCR)

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Publication history
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Acknowledgements

Publication history

Received: 30 November 2022
Revised: 06 January 2023
Accepted: 12 January 2023
Published: 27 February 2023
Issue date: October 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

We thank the National Natural Science Foundation of China (Nos. 22288101, 21920102005, and 21835002) and the 111 Project (No. B17020) for supporting this work.

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