Effect of samarium on the N2 selectivity of SmxMn0.3−xTi catalysts during selective catalytic reduction of NOx with NH3

Shengyang Zhang; Bolin Zhang; Boyu Wu; Bo Liu; Shengen Zhang

doi:10.1007/s12613-021-2348-5

Volume 30 Issue 4

Apr. 2023

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Article Navigation > International Journal of Minerals, Metallurgy and Materials > 2023 > 30(4): 642-652

Shengyang Zhang, Bolin Zhang, Boyu Wu, Bo Liu, and Shengen Zhang, Effect of samarium on the N₂ selectivity of Sm_xMn_0.3−xTi catalysts during selective catalytic reduction of NO_x with NH₃, Int. J. Miner. Metall. Mater., 30(2023), No. 4, pp. 642-652. https://doi.org/10.1007/s12613-021-2348-5

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Shengyang Zhang, Bolin Zhang, Boyu Wu, Bo Liu, and Shengen Zhang, Effect of samarium on the N2 selectivity of SmxMn0.3−xTi catalysts during selective catalytic reduction of NOx with NH3, Int. J. Miner. Metall. Mater., 30(2023), No. 4, pp. 642-652. https://doi.org/10.1007/s12613-021-2348-5

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Research Article

Effect of samarium on the N₂ selectivity of Sm_xMn_0.3−xTi catalysts during selective catalytic reduction of NO_x with NH₃

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Corresponding authors:
Bolin Zhang E-mail: zhangbolin@ustb.edu.cn

Shengen Zhang E-mail: zhangshengen@mater.ustb.edu.cn
Received: 13 April 2021; Revised: 5 September 2021; Accepted: 6 September 2021; Available online: 7 September 2021

Abstract

Abstract

This work aims to study the improvement effect of Sm on Mn-based catalysts for selective catalytic reduction (SCR) of NO with NH₃. A series of Sm_xMn_0.3−xTi catalysts (x = 0, 0.1, 0.15, 0.2, and 0.3) were prepared by co-precipitation. Activity tests indicated that the Sm_0.15Mn_0.15Ti catalyst showed superior performances, with a NO conversion of 100% and N₂ selectivity above 87% at 180–300°C. The characterizations showed that Sm doping suppressed the crystallization of TiO₂ and Mn₂O₃ phases and increased the specific surface area and acidity. In particular, the surface area increased from 152.2 m²·g⁻¹ for Mn_0.3Ti to 241.7 m²·g⁻¹ for Sm_0.15Mn_0.15Ti. These effects contributed to the high catalytic activity. The X-ray photoelectron spectroscopy (XPS) results indicated that the relative atomic ratios of Sm³⁺/Sm and O_β/O of Sm_0.15Mn_0.15Ti were 76.77at% and 44.11at%, respectively. The presence of Sm contributed to an increase in surface-absorbed oxygen (O_β) and a decrease in Mn⁴⁺ surface concentration, which improved the catalytic activity. In the results of hydrogen temperature-programmed reduction (H₂-TPR), the presence of Sm induced a higher reduction temperature and lower H₂ consumption (0.3 mmol·g⁻¹) for the Sm_0.15Mn_0.15Ti catalyst compared to the Mn_0.3Ti catalyst. The decrease in Mn⁴⁺ weakened the redox property of the catalysts and increased the N₂ selectivity by suppressing N₂O formation from NH₃ oxidation and the nonselective catalytic reduction reaction. The in situ diffuse reflectance infrared Fourier transform spectra (DRIFTs) revealed that NH₃-SCR of NO over the Sm_0.15Mn_0.15Ti catalyst mainly followed the Eley–Rideal mechanism. Sm doping increased surface-absorbed oxygen and weakened the redox property to improve the NO conversion and N₂ selectivity of the Sm_0.15Mn_0.15Ti catalyst.
- manganese oxides;
- nitric oxide;
- nitrous oxide;
- samarium;
- selective catalytic reduction;
- nitrogen selectivity

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