Revealing M (M = Cu, Co and Zr) oxides doping effects on anti-PbCl2 poisoning over Mn-Ce/AC catalysts in low-temperature NH3-SCR reaction.

Lead salts poisoning was a great challenge for the catalysts application in selective catalytic reduction (SCR) reaction of NO x with NH 3 in stationary sources. Herein, several typical transition metal (Cu, Co and Zr) oxides modified Mn-Ce/AC catalysts were prepared by impregnation method, and the effects of Cu, Co and Zr doping on resistance PbCl 2 poisoning for the catalyst were investigated. The addition of three transition metal oxides improved the PbCl 2 resistance of Mn-Ce/AC catalyst and maintained excellent low-temperature denitrification activity of the catalyst. The lead resistance performance of the three metal oxides followed: Cu > Co > Zr oxides. The NO conversion of Cu-doping catalyst after PbCl 2 poisoning was only ca. 10% lower than that of fresh Mn-Ce/AC catalyst at 225 °C. Cu, Co and Zr doping could decrease the loss of specific surface area caused by poisoning, while Cu-doped catalyst showed lowest crystallinity of active components. Meanwhile, the contents of Mn4+ and chemisorbed oxygen in Cu-doped catalyst were higher than those in Co- or Zr-doped catalysts. Cu, Co and Zr doping improved the surface acidity and redox performance of the poisoned catalysts, with Cu-doped poisoned catalyst exhibiting nearly the same surface acidity and redox performance as the fresh Mn-Ce/AC catalyst. Furthermore, Cu doping could also improve NO adsorption and was in favor to the SCR process. Besides, in situ DRIFTS results showed that the catalytic reaction pathways of all the poisoned or modified catalysts were in accordance with both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) mechanisms. Finally, a possible anti-PbCl 2 poisoning mechanistic model of (Cu, Co and Zr) oxides modified on Mn-Ce/AC catalyst was proposed. [Display omitted] • Cu-modified MC/AC catalyst showed best resistance to PbCl 2 poisoning. • Transition metal oxides alleviated damage of PbCl 2 to MC/AC structure. • Redox ability and acidity of PbCl 2 -poisoned catalyst were promoted by modifying. • NH 3 -SCR reaction on PbCl 2 -poisoned catalyst followed L-H and E-R mechanism. [ABSTRACT FROM AUTHOR]