Chinese Journal of Catalysis ›› 2018, Vol. 39 ›› Issue (4): 728-735.DOI: 10.1016/S1872-2067(17)63008-0

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Supercritical water syntheses of transition metal-doped CeO2nano-catalysts for selective catalytic reduction of NO by CO: An in situ diffuse reflectance Fourier transform infrared spectroscopy study

Xiaoxia Daia, Weiyu Jianga, Wanglong Wanga, Xiaole Wenga,b, Yuan Shanga, Yehui Xuea, Zhongbiao Wua,b   

  1. a Ministry of Education Key Laboratory of Environment Remediation and Ecological Health, College of Environmental and Resource and Sciences, Zhejiang University, Hangzhou 310058, Zhejiang, China;
    b Zhejiang Provincial Engineering Research Centre of Industrial Boiler & Furnace Flue Gas Pollution Control, Hangzhou 310058, Zhejiang, China
  • Received:2017-11-29 Revised:2017-12-26 Online:2018-04-18 Published:2018-04-08
  • Contact: 10.1016/S1872-2067(17)63008-0
  • Supported by:

    This work was supported by the National Key Research & Development Program of China (2016YFC0204100), National Natural Science Foundation of China (51478418),, and the Program for Zhejiang Leading Team of S&T Innovation (2013TD07).

Abstract:

In the present study, we synthesized CeO2 catalysts doped with various transition metals (M=Co, Fe, or Cu) using a supercritical water hydrothermal route, which led to the incorporation of the metal ions in the CeO2 lattice, forming solid solutions. The catalysts were then used for the selective catalytic reduction (SCR) of NO by CO. The Cu-doped catalyst exhibited the highest SCR activity; it had a T50 (i.e., 50% NO conversion) of only 83℃ and a T90 (i.e., 90% NO conversion) of 126℃. Such an activity was also higher than in many state-of-the-art catalysts. In situ diffuse reflectance Fourier transform infrared spectroscopy suggested that the MOx-CeO2 catalysts (M=Co and Fe) mainly followed an Eley-Rideal reaction mechanism for CO-SCR. In contrast, a Langmuir-Hinshelwood SCR reaction mechanism occurred in CuO-CeO2 owing to the presence of Cu+ species, which ensured effective adsorption of CO. This explains why CuO-CeO2 exhibited the highest activity with regard to the SCR of NO by CO.

Key words: Supercritical water, Nitrogen oxides, CO, Selective catalytic reduction, Diffuse reflectance Fourier transform infrared spectroscopy, CeO2