Effect of Ni/SiO2 catalyst preparation method on methane decomposition and CO₂ gasification cycles

Catalytic methane decomposition is a promising reaction to produce CO₂-free hydrogen from methane-rich feedstock with solid carbon as a by-product. Significant research conducted on this reaction to find ways to manage and utilize this solid carbon. In this work, the methane decomposition reaction is followed by Reverse Boudouard Reaction using CO₂ feedstock to convert the solid carbon to carbon monoxide, which is a valuable starting component for many chemical applications. Realizing this promising concept would require a catalyst that is efficient for both reactions. Herein, we explored the potential of using solution combustion synthesis (SCS) to make a 5 wt% of Ni supported SiO2 catalyst and benchmarked it versus the conventional impregnation method. The catalyst prepared by SCS showed an improved performance at different temperatures, space velocities, and catalyst pellet sizes. The SCS catalyst successfully completed five repeated cycles reaching up to 38.1 h of stable time on stream operation, whereas the impregnated catalyst was not able to complete the second testing cycle with only 14 h of time on stream operation. A thorough characterization using XRD, H₂ and O₂ TPR, TEM, SEM, XPS, and Raman spectroscopy were conducted to provide an adequate explanation for the observed performances for both catalysts. The Ni nanoparticles size and distribution, the strength of the metal support interaction, and the nature of graphitic carbon were the key factors affecting the catalytic performance. Insights on how to make an optimal catalyst for this promising process is identified which is a step forward toward making separated H₂ and CO streams from methane feedstock and CO₂, respectively.