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.
Authors
- Yan Zhang (ORCID: https://orcid.org/0000-0002-5423-8255)
- Yulong Shan (ORCID: https://orcid.org/0000-0002-5031-8522)
- Zhongbiao Wu (ORCID: https://orcid.org/0000-0003-0182-5971)
- Shan Gao (ORCID: https://orcid.org/0000-0002-5962-290X)
- Jianqi Liu (ORCID: https://orcid.org/0000-0002-6336-0084)
- Yunbo Yu (ORCID: https://orcid.org/0000-0003-2935-0955)
- Xuanhao Wu (ORCID: https://orcid.org/0000-0001-6177-6089)
- Wenpo Shan (ORCID: https://orcid.org/0000-0003-2818-5708)
- Jingyi Wang (ORCID: https://orcid.org/0000-0002-7192-533X)
- Shichao Han (ORCID: https://orcid.org/0000-0002-1153-1339)
- Jinpeng Du (ORCID: https://orcid.org/0000-0003-2699-6857)
- Hong He (ORCID: https://orcid.org/0000-0001-8476-8217)
Institutions
- 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)
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