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    Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation

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    Authors
    Liu, Jie
    Li, Xin Yong
    Zhao, Q.
    Ke, Jun
    Xiao, H.
    Lv, X.
    Liu, Shaomin
    Tadé, Moses
    Wang, Shaobin
    Date
    2017
    Type
    Journal Article
    
    Metadata
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    Citation
    Liu, J. and Li, X.Y. and Zhao, Q. and Ke, J. and Xiao, H. and Lv, X. and Liu, S. et al. 2017. Mechanistic investigation of the enhanced NH3-SCR on cobalt-decorated Ce-Ti mixed oxide: In situ FTIR analysis for structure-activity correlation. Applied Catalysis B: Environmental. 200: pp. 297-308.
    Source Title
    Applied Catalysis B: Environmental
    DOI
    10.1016/j.apcatb.2016.07.020
    ISSN
    0926-3373
    School
    Department of Chemical Engineering
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP150103026
    URI
    http://hdl.handle.net/20.500.11937/18001
    Collection
    • Curtin Research Publications
    Abstract

    A series of transition metals (Co, Cu and Fe) were selected to decorate Ce-Ti mixed oxide to elevate the low-temperature activity of selective catalytic reduction of NOx by NH3 (NH3-SCR) reaction, by adjusting the ratio of surface Ce3+ species and oxygen vacancies. Among them, Co-Ce-Ti sample exhibited the excellent low-temperature activity and broadened temperature window, which could be attributed to the improvement of the physico-chemical properties and the acceleration of the reactions in the Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. Owing to the different ionic sizes of Co2+ and Ce4+, the lattice distortion of Ce-Ti mixed oxide was greatly aggravated and subsequently increased the ratio of Ce3+ and the surface adsorbed oxygen, which benefited the generation of adsorbed NOx species and improved the reaction in the L-H mechanism. Meanwhile, the coordinatively unsaturated cationic sites over the Co-Ce-Ti sample induced more Lewis acid sites and enhanced the formation of the adsorbed NH3 species bounded with Lewis acid sites, which were considered as the crucial intermediates in E-R mechanism, and therefore facilitating the reaction between the adsorbed NH3 species and NO molecules. The enhancements in both the reactions from L-H and E-R mechanisms appeared to directly correlated with the improved deNOx performance on the Co-Ce-Ti sample, and the L-H mechanism could be the dominate one at low temperatures due to its rapid reaction rate.

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