Chinese Journal of Catalysis ›› 2018, Vol. 39 ›› Issue (4): 710-717.DOI: 10.1016/S1872-2067(18)63011-6

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The effect of cations (NH4+, Na+, K+, and Ca2+) on chemical deactivation of commercial SCR catalyst by bromides

Huazhen Changa, Chuanning Shia, Mingguan Lia, Tao Zhanga, Chizhong Wangb, Lilong Jiangc, Xiuyun Wangc   

  1. a School of Environment and Natural Resources, Renmin University of China, Beijing 100872, China;
    b State Key Joint Laboratory of Environment Simulation and Pollution Control(SKLESPC), School of Environment, Tsinghua University, Beijing 100084, China;
    c National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, Fujian, China
  • Received:2017-11-20 Revised:2017-12-28 Online:2018-04-18 Published:2018-04-08
  • Contact: 10.1016/S1872-2067(18)63011-6
  • Supported by:

    This work was supported by the National Key R&D Program of China (2016YFC0203900, 2016YFC0203901) and National Natural Science Foundation of China (51778619, 21577173).

Abstract:

Alkali and alkaline-earth metals from fly ash have a significant deactivation effect on catalysts used for selective catalytic reduction of NOx by NH3 (NH3-SCR). Bromides are considered effective additives to improve Hg0 oxidation on SCR catalysts. In this work, the effects of different bromides (NH4Br, NaBr, KBr, and CaBr2) on a commercial V2O5-WO3/TiO2 catalyst were studied. NOx conversion decreased significantly over the KBr-poisoned catalyst (denoted as L-KBr), while that over NaBr-and CaBr2-poisoned catalysts (denoted as L-NaBr and L-CaBr, respectivity) decreased to a lesser extent compared with the fresh sample. Poor N2 selectivity was observed over L-NaBr, L-KBr and L-CaBr catalysts. The decrease in the ratio of chemisorbed oxygen to total surface oxygen (Oα/(Oα + Oβ + Ow)), reducibility and surface acidity might contribute to the poor activity and N2 selectivity over L-KBr catalyst. The increased Oαratio was conducive to the enhanced reducibility of L-CaBr. Combined with enhanced surface acidity, this might offset the negative effect of the loss of active sites by CaBr2 covering. The overoxidation of NH3 and poor N2 selectivity in NH3 oxidation should retard the SCR activity at high temperatures over L-CaBr catalyst. The increased basicity might contribute to increased NOx adsorption on L-KBr and L-CaBr catalysts. A correlation between the acid-basic and redox properties of bromide-poisoned catalysts and their catalytic properties is established.

Key words: Bromide, Cation, Catalyst deactivation, SCR catalyst, N2 selectivity, Surface acidity