[논문]Low-temperature NH3-SCR catalytic characteristic of Ce-Fe solid solutions based on rare earth concentrate

Zhang, Kai; Wang, Jingjing; Guan, Pufang; Li, Na; Gong, Zhijun; Zhao, Ran; Luo, Huijuan; Wu, Wenfei

doi:10.1016/j.materresbull.2020.110871

[해외논문] Low-temperature NH3-SCR catalytic characteristic of Ce-Fe solid solutions based on rare earth concentrate

Materials research bulletin, v.128, 2020년, pp.110871 -

Zhang, Kai (School of energy and environment, Inner Mongolia University of Science & Technology) , Wang, Jingjing (School of energy and environment, Inner Mongolia University of Science & Technology) , Guan, Pufang (School of energy and environment, Inner Mongolia University of Science & Technology) , Li, Na (School of energy and environment, Inner Mongolia University of Science & Technology) , Gong, Zhijun (School of energy and environment, Inner Mongolia University of Science & Technology) , Zhao, Ran (School of energy and environment, Inner Mongolia University of Science & Technology) , Luo, Huijuan (School of energy and environment, Inner Mongolia University of Science & Technology) , Wu, Wenfei (School of energy and environment, Inner Mongolia University of Science & Technology)

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Abstract A variety of Ce-Fe solid solutions was synthesized by a microwave hydrothermal method following the molar ratio of Fe and Ce in Bayan Obo rare earth concentrate, to evaluate the catalytic action of Fe and Ce in NH3-SCR denitrification reaction. The microstructure, surface properties and catalytic activity of CeO2-Fe2O3/Al2O3 catalyst samples were characterized by NH3-SCR, SEM, BET, NH3-TPD, XRD, Raman, XPS, and DRIFTS. The results showed that the adsorption capacity of NH3 is the strongest when the molar ratio of Ce-Fe was 1:0.35, and the catalytic activity is the highest, up to 90%. The increase of iron species is beneficial to the denitration performance of the catalysts. The structure of CeO2 is distorted to form the Ce-Fe solid solutions, and more oxygen vacancies in the catalysts were exposed. Activated nitrate was generated from NO under the action of Ce3+and Fe2+, which was converted to N2 and H2O with the amide. Highlights The change of crystal phase structure during the process of Fe3+ replacing Ce4+ to form Ce-Fe solid solution facilitated the homogeneous dispersion of the active components on the catalyst surface and increased the acid sites and specific surface area of the catalyst. Excellent NH3-SCR active temperature range is the low temperature window (150-300°C). The synergistic catalysis of Ce3+, Fe2+, Oα promoted L-H mechanism, activated nitrate was generated from NO under the action of Ce3+and Fe2+, which was convert to N2 and H2O with the amide. The Ce/Fe molar ratio of 1:0.35 shows the optimal performance in terms of structure morphology, catalytic activity and surface properties. The proper increase of iron content is contributes to the catalytic activity in Bayan Obo rare earth concentrate. Graphical abstract The NH3 adsorbed by the Lewis acid sites was rapidly converted to NH2, and the Bronsted acid sites NH4 + was increased slightly, the intermediate products had higher activity on the Lewis acid and Bronsted acid sites, the reaction followed the E–R mechanism. The adsorbed NO reacts with metal ions to convert to activated nitrate, which was following the L-H mechanism. The amino intermediate was adsorbed and reacted with the activated nitrate species, eventually become N2 (Shown in Fig. 20). Microscopically, during the reduction of NO, NH3 shows selectivity to the reaction intermediates, and preferentially reacts with monodentate nitrate and bridged nitrate at low temperature. [DISPLAY OMISSION]

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[해외논문] Low-temperature NH3-SCR catalytic characteristic of Ce-Fe solid solutions based on rare earth concentrate

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