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

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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 SmxMn0.3−xTi catalysts (x = 0, 0.1, 0.15, 0.2, and 0.3) were prepared by co-precipitation. Activity tests indicated that the Sm0.15Mn0.15Ti 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 Mn0.3Ti to 241.7 m2°g−1 for Sm0.15Mn0.15Ti. 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 Oβ/O of Sm0.15Mn0.15Ti were 76.77at% and 44.11at%, respectively. The presence of Sm contributed to an increase in surface-absorbed oxygen (Oβ) 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 Sm0.15Mn0.15Ti catalyst compared to the Mn0.3Ti 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 Sm0.15Mn0.15Ti 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 Sm0.15Mn0.15Ti catalyst.

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Acknowledgements

This work was sponsored by the National Key R&D Program of China (Nos. 2021YFC1910504, 2019YFC 1907101, and 2019YFC1907103), the Key R&D Program of Ningxia Hui Autonomous Region, China (Nos. 2020BCE01001 and 2021BEG01003), the National Natural Science Foundation of China (Nos. U2002212, 51672024, 52102058, and 52204414), the Xijiang Innovation and Entrepreneurship Team (No. 2017A0109004), the Fundamental Research Funds for the Central Universities (Nos. FRF-TP-20-097A1Z and FRF-TP-20-031A1), and the Foshan Science and Technology Innovation Special Foundation (No. BK22BE001).

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Authors and Affiliations

  1. Institute for Advanced Materials and Technology, University of Science and Technology Beijing, Beijing, 100083, China

    Shengyang Zhang, Bolin Zhang, Boyu Wu, Bo Liu & Shengen Zhang

  2. Shunde Innovation School, University of Science and Technology Beijing, Foshan, 528399, China

    Bolin Zhang

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Zhang, S., Zhang, B., Wu, B. et al. 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, 642–652 (2023). https://doi.org/10.1007/s12613-021-2348-5

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