Towards rational design of Cu-SSZ-13 catalysts with less N2O formation in NH3-SCR reaction: The effect of Brønsted acid sites

Ammonia Selective Catalytic Reduction (NHs-SCR) technology has been employed to eliminate NO<sub>x</sub> from diesel engine exhaust, with Cu-SSZ-13 serving as the commercial catalyst. The greenhouse gas N<sub>2</sub>O is produced as a byproduct when using Cu-SSZ-13 as the NH<sub>3</sub>-SCR catalyst. To achieve synergistic control of pollutants and greenhouse gases in diesel engine exhaust, rational design of Cu-SSZ-13 catalysts is required. In this study, the effect of Brønsted acid sites in Cu-SSZ-13 catalysts on the formation of N<sub>2</sub>O was investigated. Mild thermal treatment was innovatively employed to prepare Cu-SSZ-13 catalysts with different amounts of Brønsted acid sites. EPR, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD, NMR were utilized to determine that the Brønsted acid sites were modified while the Cu species remained unchanged. Thereby an accurate assessment of the influence of Brønsted acid sites on N<sub>2</sub>O formation could be achieved. Our results showed that Cu-SSZ-13 with more Brønsted acid sites produced less N<sub>2</sub>O during the NH<sub>3</sub>-SCR reaction. In the low-temperature region, the presence of framework acid sites facilitates the decomposition of the NH<sub>4</sub>NO<sub>3</sub> assisted by NO to form N<sub>2</sub> and H<sub>2</sub>O, reducing the formation of N<sub>2</sub>O. In the high-temperature region, the Brønsted acid sites promote the decomposition of NH<sub>2</sub>NO into N<sub>2</sub> and H<sub>2</sub>O. Meanwhile, the N<sub>2</sub>O-SCR reaction can also be promoted by Brønsted acid sites, thereby decreasing N<sub>2</sub>O emissions. This study suggests that in the future design and synthesis of Cu-SSZ-13 zeolites, attention should be paid to creating more Brønsted acid sites in Cu-SSZ-13 to reduce N<sub>2</sub>O emissions.

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Publication Details

Journal
Journal of Environmental Sciences
Published
2024-12-06
DOI
https://doi.org/10.1016/j.jes.2024.12.001
Citations
8
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.94
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article

Towards rational design of Cu-SSZ-13 catalysts with less N2O formation in NH3-SCR reaction: The effect of Brønsted acid sites

Yan Zhang, Yulong Shan, Zhongbiao Wu, Shan Gao et al.
8 citations
Journal of Environmental Sciences
Catalytic Processes in Materials Science
0.94
article

Towards rational design of Cu-SSZ-13 catalysts with less N2O formation in NH3-SCR reaction: The effect of Brønsted acid sites

Yan Zhang, Yulong Shan, Zhongbiao Wu, Shan Gao, Jianqi Liu, Yunbo Yu, Xuanhao Wu, Wenpo Shan, Jingyi Wang, Shichao Han, Jinpeng Du, Hong He
article en
8 citations

Abstract

Ammonia Selective Catalytic Reduction (NHs-SCR) technology has been employed to eliminate NO<sub>x</sub> from diesel engine exhaust, with Cu-SSZ-13 serving as the commercial catalyst. The greenhouse gas N<sub>2</sub>O is produced as a byproduct when using Cu-SSZ-13 as the NH<sub>3</sub>-SCR catalyst. To achieve synergistic control of pollutants and greenhouse gases in diesel engine exhaust, rational design of Cu-SSZ-13 catalysts is required. In this study, the effect of Brønsted acid sites in Cu-SSZ-13 catalysts on the formation of N<sub>2</sub>O was investigated. Mild thermal treatment was innovatively employed to prepare Cu-SSZ-13 catalysts with different amounts of Brønsted acid sites. EPR, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD, NMR were utilized to determine that the Brønsted acid sites were modified while the Cu species remained unchanged. Thereby an accurate assessment of the influence of Brønsted acid sites on N<sub>2</sub>O formation could be achieved. Our results showed that Cu-SSZ-13 with more Brønsted acid sites produced less N<sub>2</sub>O during the NH<sub>3</sub>-SCR reaction. In the low-temperature region, the presence of framework acid sites facilitates the decomposition of the NH<sub>4</sub>NO<sub>3</sub> assisted by NO to form N<sub>2</sub> and H<sub>2</sub>O, reducing the formation of N<sub>2</sub>O. In the high-temperature region, the Brønsted acid sites promote the decomposition of NH<sub>2</sub>NO into N<sub>2</sub> and H<sub>2</sub>O. Meanwhile, the N<sub>2</sub>O-SCR reaction can also be promoted by Brønsted acid sites, thereby decreasing N<sub>2</sub>O emissions. This study suggests that in the future design and synthesis of Cu-SSZ-13 zeolites, attention should be paid to creating more Brønsted acid sites in Cu-SSZ-13 to reduce N<sub>2</sub>O emissions.

Journal of Environmental SciencesVol. 157
Chinese Academy of Sciences (CN), Shanghai Advanced Research Institute (CN), Institute of Urban Environment (CN), State Key Joint Laboratory of Environment Simulation and Pollution Control (CN), Research Center for Eco-Environmental Sciences (CN), Chinese Research Academy of Environmental Sciences (CN), Zhejiang University (CN)
Openalex Percentile: Top 22%
Catalytic Processes in Materials Science
0.94
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