Sulfated CeO cubes were prepared by the impregnation of CeO cubes by ammonium sulfates, and further evaluated in selective catalytic reduction of NO with ammonia (NH-SCR). Catalytic activity tests indicated that NO reduction conversions and N selectivity of sulfated CeO cubes could be significantly improved compared to pure CeO cubes. The synthesized sulfated CeO cubes were further characterized by atom-resolved high angle annular dark-field (HAADF) imaging, Fourier-transform infrared spectroscopy (FTIR) by pyridine adsorption, and temperature-programmed reduction by H (H-TPR). The characterization results showed that sulfates were primarily dispersed through the corners, edges, and surfaces of CeO cubes, and did not significantly affect the crystal structures of CeO cubes. Sulfation treatment could create and strengthen Brønsted acid sites originated from the protons on surface sulfates, further facilitating ammonia adsorption and activation. The kinetic data indicated that the apparent reaction order of NO, O, and NH was 0.95 to 1.01, -0.01 to 0.00, and -0.18 to -0.15, respectively. It could speculate that gaseous phase NO involving in NO catalytic oxidation was the rate-determining step over sulfated CeO cubes for NH-SCR reaction. The presence of NH slightly inhibited the SCR reaction rate due to the competitive adsorption blocking NO oxidation sites.

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http://dx.doi.org/10.1016/j.jhazmat.2021.126545DOI Listing

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