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Selective catalytic reduction of NOx with NH3 over Mn–Zr–Ti mixed oxide catalysts

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Abstract

Mixed oxide catalysts yMn–Zr–Ti (y/10/10 with y = 1, 3, 5, 7 and 9) for the selective catalytic reduction (SCR) of NOx with NH3 in the presence of oxygen were synthesized by co-precipitation. The catalyst 5Mn–Zr–Ti exhibited a catalytic activity higher than 87% above 160 °C and N2 selectivity above 92% at 100–300 °C. The SCR performance was quite stable at 180 and 200 °C for 15 h. Mn species are shown to improve the catalytic activity by providing more surface labile oxygen, while a synergistic effect among Mn, Zr and Ti species suppressed the generation of N2O. According to in situ DRIFT analysis, NOx was primarily reduced by the reaction of bidentate nitrate and monodentate nitrito species with adsorbed NH3. Subsequently, a comprehensive reaction mechanism was proposed. Accordingly, the formation of NH species was inhibited, and hence, the N2O formation by the reaction of NH and bidentate nitrate was suppressed. Furthermore, the investigation of the deactivation mechanism by SO2 indicated that both the deposition of ammonium sulfates and the sulfation of Mn active sites resulted in the deactivation of the catalyst 5Mn–Zr–Ti. The deposition of ammonium sulfates at 180 °C was more pronounced than that at 220 °C.

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Acknowledgements

This work is sponsored by the National Natural Science Foundation of China (Grants U1360202, 51672024, 51472030 and 51502014) and the Fundamental Research Funds for the Central Universities (2302017FRF-IC-17-005 and 2302017FRF-BR-17-005A).

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

    Bolin Zhang, Bo Liu, Lin Li & Shengen Zhang

  2. Institute of Chemical Technology, Leipzig University, 04103, Leipzig, Germany

    Michael Liebau & Roger Gläser

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Zhang, B., Liebau, M., Liu, B. et al. Selective catalytic reduction of NOx with NH3 over Mn–Zr–Ti mixed oxide catalysts. J Mater Sci 54, 6943–6960 (2019). https://doi.org/10.1007/s10853-019-03369-z

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