Insight into the role of preparation method on the structure and size effect of Ni/MSS catalysts for dry reforming of methane

Dry reforming of methane (DRM) is considered a promising process to convert CH4 and CO2 into syngas for achieving carbon neutrality. However, sintering and carbon deposition of Ni pose significant challenges to the industrialization of DRM. The size of Ni particles significantly affects the generation of carbon deposits. In this study, a series of Ni/MSS catalysts were prepared using four different methods, including common impregnation, glycine-assisted impregnation, ethylene glycol-assisted impregnation and ammonia evaporation. The effects of preparation methods on the anti-sintering and anti-coking properties were explored through various characterization techniques. Results showed that glycine-assisted impregnation and ethylene glycol-assisted impregnation effectively improved the dispersion of Ni, resulting in small Ni particles while preserving the unique pore structure of MSS supports. Smaller Ni particles expose more active sites, which facilitate the resistance to carbon accumulation. These catalysts show the highest activity and excellent stability. The catalyst prepared by ammonia evaporation showed the best stability due to the synergistic effect of the strongest basicity and metal-support interaction. However, nickel phyllosilicate generation consumed a small amount of MSS, resulting in reduced specific surface area. Compared with the common impregnation method, the other three methods reduced the particle size of Ni and improved the interaction between support and metal, effectively enhancing the ability of the catalyst to resist coking and sintering. Kinetic studies also showed a significant decrease in the apparent activation energy of methane and carbon dioxide cracking due to the reduced particle size of Ni particles.