Applied Catalysis A: General, Vol.230, No.1-2, 177-193, 2002
Sulfur- and water-tolerance of Pt/KL aromatization catalysts promoted with Ce and Yb
Different Pt/KL catalysts containing rare earth (RE; Ce and Yb) promoters were prepared by two techniques, incipient wetness impregnation (IWI) and vapor phase impregnation (VPI). The catalysts were tested for the activity and the selectivity of n-hexane aromatization to benzene under clean, sulfur-containing, and water-containing feeds at 500 degreesC. It was observed that the catalysts prepared by the VPI technique exhibited much higher activity and selectivity than those prepared by M. It was also found that although under clean conditions, the addition of Ce or Yb caused a decrease in activity, in the presence of sulfur the addition of Ce and to a lesser extent Yb, significantly inhibited catalyst deactivation. The influence of water in the feed was investigated by contacting the catalysts for 1 h to a feed containing 3 mol.% water. After this treatment, all the catalysts exhibited a significant activity loss. This loss was more pronounced for the catalyst prepared by the VPI method. The catalyst prepared by M already had suffered a significant deactivation before the water treatment, so the activity drop was not so pronounced. The sample prepared by VPI not only showed a drop in activity immediately after the water treatment but it became more susceptible to deactivation afterwards. By contrast, the Ce-promoted catalyst showed a more stable activity after the water treatment. All catalysts were characterized before and after reaction by a number of techniques. In agreement with previous studies, FT-IR of adsorbed CO and chemisorption results indicated that the VPI method resulted in higher Pt dispersion than that obtained by the IWI method. After reaction in the presence of sulfur, the Ce-promoted Pt/KL catalyst showed a higher resistance to metal agglomeration and a lower rate of coke formation than the unpromoted Pt/KL. On all the catalysts, the amount of carbon deposits was greater in the presence of sulfur and after exposure to water vapor than under the reaction with clean feeds. This difference is explained in terms of metal particle growth and location in the zeolite.
Keywords:n-hexane aromatization;Pt/KL zeolite;VPI method;sulfur-tolerance;hydrothermal stability;cerium promoter;ytterbium promoter;DRIFTS;XANES;TPO