Study on the Anti-Coking Nature of Ni/SrTiO3 Catalysts by the CH4 Pyrolysis

Abstract

A solid phase crystallization (spc) method was applied for the preparation of SrTiO3-supported Ni catalysts and compared to the impregnation (imp) method. spc-Ni0.2/SrTiO3 has highly dispersed and stable Ni metal particles resulting in higher activity and higher sustainability against coking than imp-Ni0.2/SrTiO3 in the partial oxidation of CH4. Both catalysts were tested for the CH4 pyrolysis in order to elucidate the catalytic nature against coking of spc-Ni0.2/SrTiO3. The amount of carbon and the rate of H2 formation were similar over both catalysts at both 773 and 1073 K. On both catalysts, CH4 continuously decomposed at 773 K, while the rate of CH4 pyrolysis quickly decreased at 1073 K. Fibrous carbons grew up with a Ni metal particle on the tip of the fiber at 773 K, while carbon balls and short carbon fibers with a Ni metal particle encapsulated inside formed and no sufficient growth of the fiber was observed at 1073 K. The carbon species formed at 773 K was hydrogenated completely to CH4 around 873 K, while the hydrogenation of that formed at 1073 K needed higher temperature around 1073 K. However, the carbon species formed on both the catalysts at either 773 or 1073 K was completely oxidized around 773 K. Thus, judging from the anti-coking nature, the behaviors in the CH4 pyrolysis are similar over both catalysts, nonetheless spc-Ni0.2/SrTiO3 was far superior to imp-Ni0.2/SrTiO3 in the CH4 oxidation. It is likely that the high sustainability against coking of spc-Ni0.2/SrTiO3 is not due to its intrinsic nature suppressing the coking but due to its high activity of reforming which can quickly eliminate the carbon formed on the catalyst surface.