Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (8): 1314-1323.DOI: 10.1016/S1872-2067(15)61115-9

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Fe-Mn/Al2O3 catalysts for low temperature selective catalytic reduction of NO with NH3

Xiaobo Wanga,b, Shiguo Wua,b, Weixin Zoua,b, Shuohan Yua,b, Keting Guic, Lin Donga,b   

  1. a. Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China;
    b. Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Nanjing University, Nanjing 210093, Jiangsu, China;
    c. Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, Jiangsu, China
  • Received:2016-03-03 Revised:2016-04-18 Online:2016-07-29 Published:2016-08-01
  • Contact: Xiaobo Wang, Lin Dong
  • Supported by:

    This work was supported by the National High Technology Research and Development Program of China (863 Program, 2015AA03A401), the National Natural Science Foundation of China (51276039), the Fundamental Research Funds for the Central Universities (020514380020, 020514380030), and the Postdoctoral Science Foundation of Jiangsu Province, China (1501033A).

Abstract:

A series of Fe-Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed-bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption-desorption, X-ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature-programmed reduction, NH3 temperature-programmed desorption, X-ray photoelectron spectroscopy (XPS), thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to characterize the catalysts. The 8Fe-8Mn/Al2O3 catalyst gave 99% of NO conversion at 150 ℃ and more than 92.6% NO conversion was obtained in a wide low temperature range of 90-210 ℃. XPS analysis demonstrated that the Fe3+ was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4+/Mn3+ ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe-8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe-8Mn/Al2O3 catalyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst.

Key words: Nitrogen monoxide, Low-temperature selective catalytic reduction, Fe-Mn catalyst, X-ray photoelectron spectroscopy, Sulfur dioxide, Fourier transform infrared spectroscopy