Chemical deactivation of V2O5/WO3-TiO2 SCR catalysts by additives and impurities from fuels, lubrication oils, and urea solution - I. Catalytic studies

摘要

The influence of the combustion products of different lubrication oil additives (Ca, Mg, Zn, P, B, Mo) and impurities in Diesel fuel (K from raps methyl ester) or urea solution (Ca, K) on the activity and selectivity of vanadia-based SCR catalysts were investigated. Standard V2O5/WO3-TiO2 catalysts coated on metal substrates (400 cpsi) were impregnated with water soluble compounds of these elements and calcined at 400 and 550 degrees C, in order to investigate the chemical deactivation potential of different elements and combinations of them. It was found that potassium strongly reduced the adsorption equilibrium constant K-NH3 of ammonia. At small ammonia concentrations in the feed, only part of the active sites were covered with ammonia resulting in a reduced SCR reaction rate. At high ammonia concentrations, the surface coverage and SCR reaction rate increased, but high SCR activity at concurrent low ammonia emissions was impossible. Calcium caused less deactivation than potassium and did not affect the ammonia adsorption to the same extent, but it lowered the intrinsic SCR reaction rate. Moreover, deactivation by calcium was much reduced if counter-ions of inorganic acids were present (order of improvement: SO42- > PO43- > BO33-). Zinc was again less deactivating than calcium, but the positive effect of the counter-ions was weaker than in case of calcium. The degree of N2O production at T > 500 degrees C, which is typical for V2O5/WO3-TiO2 catalysts, was not influenced by the different compounds, except for molybdenum, which induced a small increase in N2O formation. (C) 2007 Elsevier B.V. All rights reserved.