Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeOx catalyst for low-temperature selective catalytic reduction of NOx by ammonia

doi:10.1016/j.cjche.2024.03.012

中国化学工程学报 ›› 2024, Vol. 71 ›› Issue (7): 272-282.DOI: 10.1016/j.cjche.2024.03.012

Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_x catalyst for low-temperature selective catalytic reduction of NO_x by ammonia

Qiyao Zhang, Shuangshuang Zhang, Xu Hu, Yongmin Huang

Key Laboratory of Specially Functional Polymeric Materials and Related Technology, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

收稿日期:2023-11-18 修回日期:2024-03-10 出版日期:2024-07-28 发布日期:2024-08-30
通讯作者: Yongmin Huang,E-mail:huangym@ecust.edu.cn
基金资助:
This research was supported by the Fundamental Research Funds for the Central Universities (222201817001) and Shanghai Sailing Program (21YF140800). Research Centre of Analysis and Test of ECUST provided analysis assistance.

Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_x catalyst for low-temperature selective catalytic reduction of NO_x by ammonia

Qiyao Zhang, Shuangshuang Zhang, Xu Hu, Yongmin Huang

Key Laboratory of Specially Functional Polymeric Materials and Related Technology, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2023-11-18 Revised:2024-03-10 Online:2024-07-28 Published:2024-08-30
Contact: Yongmin Huang,E-mail:huangym@ecust.edu.cn
Supported by:
This research was supported by the Fundamental Research Funds for the Central Universities (222201817001) and Shanghai Sailing Program (21YF140800). Research Centre of Analysis and Test of ECUST provided analysis assistance.

摘要/Abstract

摘要： The self-made MnFeO catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction (SCR) by NH₃. In this work, the surface properties of the series of MnFe-based catalysts were studied. The results indicate Sm-modified catalyst have superior low-temperature SCR activity; NO_x conversion maintained at nearby to 100% at 90 °C to 240 °C. In addition, The N₂ selectivity of Sm doping remains above 80% in the range of 60 °C to 150 °C. In SO₂ poisoning test, the NO_x conversion can be remained >90% after 10 h of reaction. The XPS, NH₃-TPD and H₂-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer electrons. In situ diffuse reflaxions infrared Fourier transformations spectroscopy (DRIFTS) results show that NO_x is more easily adsorbed on the surface after Sm doping, which provided favorable conditions for the NH₃-SCR reaction to proceed. The reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.

关键词: SCR, Sm doping, Catalyst, Sulfur resistance, In situ DRIFTS, Selectivity

Abstract: The self-made MnFeO catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction (SCR) by NH₃. In this work, the surface properties of the series of MnFe-based catalysts were studied. The results indicate Sm-modified catalyst have superior low-temperature SCR activity; NO_x conversion maintained at nearby to 100% at 90 °C to 240 °C. In addition, The N₂ selectivity of Sm doping remains above 80% in the range of 60 °C to 150 °C. In SO₂ poisoning test, the NO_x conversion can be remained >90% after 10 h of reaction. The XPS, NH₃-TPD and H₂-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer electrons. In situ diffuse reflaxions infrared Fourier transformations spectroscopy (DRIFTS) results show that NO_x is more easily adsorbed on the surface after Sm doping, which provided favorable conditions for the NH₃-SCR reaction to proceed. The reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.

Key words: SCR, Sm doping, Catalyst, Sulfur resistance, In situ DRIFTS, Selectivity

Qiyao Zhang, Shuangshuang Zhang, Xu Hu, Yongmin Huang. Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_x catalyst for low-temperature selective catalytic reduction of NO_x by ammonia[J]. 中国化学工程学报, 2024, 71(7): 272-282.

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Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_x catalyst for low-temperature selective catalytic reduction of NO_x by ammonia

Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_x catalyst for low-temperature selective catalytic reduction of NO_x by ammonia

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