Application of calcined layered double hydroxides as catalysts for abatement of N2O emissions

Abstract

The results of catalytic decomposition of N2O over mixed oxide catalysts obtained by calcination of layered double hydroxides (LDHs) are summarized. Mixed oxides were prepared by thermal treatment (500 °C) of coprecipitated LDH precursors with general chemical composition of MII1-xMIIIx(OH)2(CO3)x/2·yH2O, where MII was Ni, Co, Cu and/or Mg, MIII was Mn, Fe and/or Al, and the MII/MIII molar ratio was adjusted to 2. The influence of chemical composition of the MII-MIII mixed oxide catalysts on their activity and stability in N2O decomposition was examined. The highest N2O conversion was reached over Ni-Al (4:2) and Co-Mn-Al (4:1:1) catalysts. Their suitability for practical application was proved in simulated process stream in the presence of O2, NO, NO2 and H2O. It was found that N2O conversion decreased with increasing amount of oxygen in the feed. The presence of NO in the feed caused a slight decrease in N2O conversion. A strong decrease in the reaction rate was observed over the Ni-Al catalyst in the presence of NO2 while no N2O conversion decrease was observed over the Co-Mn-Al catalyst. Water vapor inhibited the N2O decomposition over all tested catalysts. The obtained kinetic data for N2O decomposition in a simulated process stream over the Co-Mn-Al catalyst were used for a preliminary reactor design. The packed bed volume necessary for N2O emission abatement in a HNO3 production plant was calculated as 35 m3 for waste gas flow rate of 30 000 m3 h-1.