4.7 Article

Enhanced low-temperature activity and huimid-SO2 resistance of MnFe-based multi-oxide catalysts for the marine NH3-SCR reaction

Journal

JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
Volume 123, Issue -, Pages 209-219

Publisher

ELSEVIER SCIENCE INC
DOI: 10.1016/j.jiec.2023.03.036

Keywords

Marine emission; Manganese oxide; Doping; SCR; Sulfur-resistant

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Several MnFe-based multi-metal oxides were synthesized as NH3-SCR catalysts for reducing NOx emissions of marine diesel exhausts. The Co and Nb-doped MnFeCeAl catalysts showed high NOx conversion and N2 selectivity, and the MnFeCeAlCo catalysts inhibited sulfate species growth in humid-SO2 gases. The doping of Co, Nb, Sm, and Sb enhanced interactions among different components, promoted active component dispersion, improved redox properties and surface acidity, and raised the atomic ratios of high-valent Mn species and surface adsorbed oxygen, resulting in excellent SCR performance and humid-SO2 resistance.
Several MnFe-based multi-metal oxides were synthesized as NH3-SCR catalysts by a simple coprecipita-tion method for abating NOx of marine diesel exhausts. The Co and Nb-doped MnFeCeAl catalysts exhibit NOx conversion over 90% and N-2 selectivity above 95% at 180-270 degrees C, especially the MnFeCeAlCo cata-lysts can inhibit nearly all sulfate species growth within 150 ppm humid-SO2 gases at 225 degrees C. The struc-tural characterization results revealed that Co, Nb, Sm, and Sb doping can enhance interactions among different components and promote active component dispersion. Temperature programmed analysis indicated that the Co doping is not only more favorable for improving redox properties, but can also enhance the surface acidity, which are advantageous to improve the activity, N-2 selectivity, and humid-SO2 resistance. Moreover, the XPS results implied that the binding energy shift or the valence vari-ation of the Sm, Sb, Nb, and Co species on catalyst surfaces are favored to raise the atomic ratios of high-valent Mn species and surface adsorbed oxygen, which can promote the redox property significantly and further facilitate SCR activity. Accordingly, the excellent activity and humid-SO2 tolerance of the MnFeCeAlCo catalyst should attribute to its lower redox temperature, strong interaction between oxides, 47.3% surface Mn4+/Mn3+ species, and 71.8% adsorbed oxygen, which provide a method for improving the SCR performances of MnFe-based catalysts with humid SO2 resistance. (c) 2023 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.

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