Effect of Preparation Method on Catalytic Performance of Fe-Cu-ZSM-5 for Selective Catalytic Reduction of NOx by NH3
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Graphical Abstract
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Abstract
Nitrogen oxides is one of the major pollutants in diesel exhaust, which has caused serious environmental pollution. The selective catalytic reduction (SCR) is the most efficient way to control NOx emission, and the key is the catalysts with high activity. Recently, zeolites-based catalysts have been attracted more attention because of their special pore structure and catalytic performance. In this paper, impregnation, liquid-state ion exchange, and liquid-state ion exchange followed by impregnation methods were employed to prepare Fe-Cu-ZSM-5 catalyst. Over 80% of NO conversion can be achieved at the temperature region of 188-530℃, 200-520℃, and 240-530℃ for catalyst Fe0.7-Cu0.97-ZSM-5(IWI), Fe0.59-Cu1.0-ZSM-5(IE) and Fe0.65(IWI)-Cu0.95(IE)-ZSM-5, respectively. It was found that the catalyst Fe0.7-Cu0.97-ZSM-5 prepared with impregnation method exhibited the best catalytic performance for SCR reaction. However, the Fe0.65-Cu0.95-ZSM-5 catalyst prepared with liquid-state ion exchange followed by impregnation exhibited the lowest catalytic performance. The catalysts were characterized by XRD, UV-vis, H2-TPR, XPS, NH3-TPD, and NO oxidation. It was revealed that the catalyst Fe0.7-Cu0.97-ZSM-5(IWI) had more isolated Cu2+ and Fe3+ species at the exchange site, which are the active species for NH3-SCR reaction at the low-temperature region. In addition, the catalyst Fe0.7-Cu0.97-ZSM-5(IWI) had the stronger redox ability and NO oxidation ability, as well as more acid sites on catalyst surface compared with catalyst Fe0.59-Cu1.0-ZSM-5(IE) and Fe0.65 (IWI)-Cu0.95 (IE)-ZSM-5. Above all, the states of active Cu and Fe species, reducibility of the catalyst and acidic properties on the catalyst surface are the critical factors for the catalytic performance of the Fe-Cu-ZSM-5 catalysts.
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