Reactivation of severely aged commercial three-way catalysts by washing with weak EDTA and oxalic acid solutions

Abstract

Ethylene diamine tetraacetic acid (EDTA) which is a well-known reagent for its metal extraction efficiency was studied for the first time towards the improvement of the catalytic activity and oxygen storage and release properties (OSC) of severely aged commercial three-way catalysts (TWC) on a laboratory scale. Optimization of the experimental parameters of EDTA-washing procedure of TWC was carried out by varying the washing time, volumetric flow rate, and temperature of EDTA solution. The EDTA-washing procedure of TWC was compared with that of oxalic acid-washing regarding their efficiency in removing P, Pb, S, Ca, Zn, Fe, Cu, Cr, Ni, and Mn, all known TWC contaminants that many of them cause severe deterioration of TWC's activity and oxygen storage and release properties. EDTA appears to be significantly efficient in removing Pb, Zn, Ca, Mn, Fe, Cu and Ni metal contaminants and sulfur but not of phosphorus (P). Phosphorus-containing species were found to be efficiently removed from the aged TWCs after oxalic acid washing. All regeneration procedures applied led to a significant partial recovery of catalytic activity of TWC (CO, CxHy and NOx conversions) under real exhaust gas conditions (dynamometer tests) due to the removal of large amounts of contaminants accumulated on the aged TWC. The washing procedures using oxalic acid alone or in combination with EDTA led to more significant improvements of both catalytic and OSC performance compared with those of EDTA washing alone. This was due to the ability of oxalic acid to remove P-containing compounds which appear to be one of the main causes of commercial three-way catalyst deactivation.