Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH<sub>3</sub>-SCR

doi:10.1007/s11705-022-2258-8

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (5) : 617-633 https://doi.org/10.1007/s11705-022-2258-8

RESEARCH ARTICLE

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH₃-SCR

Junlin Xie^1,³, Yanli Ye^1,³, Qinglei Li^1,³, Tianhong Kang^1,³, Sensheng Hou^1,³, Qiqi Jin^1,³, Feng He^1,³, De Fang^1,²(

)

¹. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China
². Center for Materials Research and Analysis, Wuhan University of Technology, Wuhan 430070, China
³. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

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Abstract

MnO_x and Sm–Mn catalysts were prepared with the coprecipitation method, and they showed excellent activities and sulfur resistances for the selective catalytic reduction of NO_x by NH₃ between 50 and 300 °C in the presence of excess oxygen. 0.10Sm–Mn catalyst indicated better catalytic activity and sulfur resistance. Additionally, the Sm doping led to multi-aspect impacts on the phases, morphology structures, gas adsorption, reactions process, and specific surface areas. Therefore, it significantly enhances the NO conversion, N₂ selectivity, and sulfur resistance. Based on various experimental characterization results, the reaction mechanism of catalysts and the effect of SO₂ on the reaction process about the catalysts were extensively explored. For 0.10Sm–Mn catalyst, manganese sulfate and sulfur ammonium cannot be generated broadly under the influence of SO₂ and the amount of surface adsorbed oxygen. The Bronsted acid sites strengthen significantly due to the addition of SO₂, enhancing the sulfur resistance of the 0.10Sm–Mn catalyst.

Keywords MnO_x Sm–Mn catalyst NH₃-SCR sulfur resistance

Corresponding Author(s): De Fang

About author:

*These authors equally shared correspondence to this manuscript.

Online First Date: 03 March 2023 Issue Date: 28 April 2023

Cite this article:

Junlin Xie,Yanli Ye,Qinglei Li, et al. Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH₃-SCR[J]. Front. Chem. Sci. Eng., 2023, 17(5): 617-633.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2258-8
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I5/617

Fig.1 Performances of catalysts with different Sm content: (a) SCR activity; (b) N₂ selectivity; (c) sulfur resistance at 160 °C.

Fig.2 XRD patterns of catalysts: (a) MnO_x before poisoning; (b) MnO_x after poisoning; (c) 0.10Sm–Mn before poisoning; (d) 0.10Sm–Mn after poisoning.

Fig.3 TG-DTG diagrams of MnO_x and 0.10Sm–Mn catalysts: (a) MnO_x before poisoning; (b) MnO_x after poisoning; (c) 0.10Sm–Mn before poisoning; (d) 0.10Sm–Mn after poisoning.

Tab.1 Surface atomic concentration and relative concentration ratios by XPS

Fig.4 O1s spectra of catalysts: (a) 0.10Sm–Mn after poisoning, (b) 0.10Sm–Mn before poisoning, (c) MnO_x after poisoning, (d) MnO_x before poisoning; S2p spectra of catalysts: (e) 0.10Sm–Mn after poisoning, (f) MnO_x after poisoning.

Fig.5 SEM images of MnO_x and 0.10Sm–Mn catalysts: (a) MnO_x before poisoning; (b) MnO_x after poisoning; (c) 0.10Sm–Mn before poisoning; (d) 0.10Sm–Mn after poisoning.

Tab.2 Surface area and pore structure of MnO_x and 0.10Sm–Mn catalysts before and after poisoning

Fig.6 NH₃-TPD profiles of MnO_x and 0.10Sm–Mn catalysts before and after poisoning.

Fig.7 H₂-TPR profiles of MnO_x and 0.10Sm–Mn catalysts before and after poisoning.

Fig.8 Adsorption of reaction gases on MnO_x catalyst surface: (a) NH₃; (b) NH₃ and O₂; (c) NH₃, O₂ and NO.

Fig.9 Adsorption of reaction gases on MnO_x catalyst surface: (a) NO; (b) NO and O₂; (c) NO, O₂ and NH₃.

Fig.10 Adsorption of reaction gases on 0.10Sm–Mn catalyst surface: (a) NH₃; (b) NH₃ and O₂; (c) NH₃, O₂ and NO.

Fig.11 Adsorption of reaction gases on 0.10Sm–Mn catalyst surface: (a) NO; (b) NO and O₂; (c) NO, O₂ and NH₃.

Fig.12 (a) DRIFT results of NH₃ absorption for poisoned MnO_x poisoned by SO₂; (b) DRIFT results of NH₃ absorption for poisoned 0.10Sm–Mn poisoned by SO₂; (c) infrared spectra of NH₃ absorption for 30 min of fresh (1) and SO₂ poisoned (2) 0.10Sm–Mn catalysts.

Fig.13 (a) DRIFT results of NO absorption for poisoned MnO_x poisoned by SO₂; (b) DRIFT results of NO absorption for poisoned 0.10Sm–Mn poisoned by SO₂; (c) infrared spectra of NO absorption for 30 min of fresh (1) and SO₂ poisoned (2) 0.10Sm–Mn catalysts.

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