Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (8): 1354-1361.DOI: 10.1016/S1872-2067(15)61102-0

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Promotional effects of Zr on K+-poisoning resistance of CeTiOx catalyst for selective catalytic reductionof NOx with NH3

Baoqiang Xua, Haidi Xub,c, Tao Lina, Yi Caoa, Li Lana, Yuanshan Lid, Xi Fengd, Maochu Gonga, Yaoqiang Chena,c   

  1. a. Key Laboratory of Green Chemistry & Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, Sichuan, China;
    b. Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610064, Sichuan, China;
    c. Sichuan Provincial Environmental Protection Environmental Catalytic Materials Engineering Technology Center, Chengdu 610064, Sichuan, China;
    d. College of Chemical Engineering, Sichuan University, Chengdu 610064, Sichuan, China
  • Received:2016-02-27 Revised:2016-04-02 Online:2016-07-29 Published:2016-08-01
  • Contact: Haidi Xu, Yaoqiang Chen
  • Supported by:

    This work was supported by the Major Research Program of Sichuan Province Science and Technology Department (2012FZ0008), the National Natural Science Foundation of China (21173153), the National High Technology Research and Development Program of China (863 Program, 2013AA065304), and the Sichuan University Research Foundation for Young Teachers (2015SCU11056).

Abstract:

CeTiOx and CeZrTiOx catalysts were prepared by a coprecipitation method and used for selective catalytic reduction of NOx by NH3 (NH3-SCR). Various amounts of KNO3 were impregnated on the catalyst surface to investigate the effects of Zr addition on the K+-poisoning resistance of the CeTiOx catalyst. The NH3-SCR performance of the catalysts showed that the NOx removal activity of the Zr-modified catalyst after poisoning was better than that of the CeTiOx catalyst. Brunauer-Emmett-Teller data indicated that the Zr-containing catalyst had a larger specific surface area and pore volume both before and after K+ poisoning. X-ray diffraction, Raman spectroscopy, and transmission electron microscopy showed that Zr doping inhibited anatase TiO2 crystal grain growth, i.e., the molten salt flux effect caused by the loaded KNO3 was inhibited. The Ce 3d X-ray photoelectron spectra showed that the Ce3+/Ce4+ ratio of CeZrTiOx decreased more slowly than that of CeTiOx with increasing K+ loading, indicating that Zr addition preserved more crystal defects and oxygen vacancies; this improved the catalytic performance. The acidity was a key factor in the NH3-SCR performance; the temperature-programmed desorption of NH3 results showed that Zr doping inhibited the decrease in the surface acidity. The results suggest that Zr improved the K+-poisoning resistance of the CeTiOx catalyst.

Key words: Cerium-titanium mixed oxide, Zirconium, Potassium-poisoning resistance, Selective catalytic reduction, Nitrogen oxides