Designing highly active hydrotalcite-derived NiAl catalysts for methane cracking to H2

Abstract

Designing nickel-based methane cracking catalysts with excellent catalytic activity and surveying their transition during the catalytic process with varied reaction condition have been challenge. In this paper, NiAl catalysts were prepared by reduced hydrotalcite precursor for efficient catalytic methane cracking to produce hydrogen. The catalysts were characterized by XRD, N2 physisorption, XPS, SEM, TEM, Raman and TGA. The effects of preparation method, Ni/Al ratio and reaction temperature on methane cracking performance were revealed and the transformation for the Ni particles during the reaction process was analyzed. The results indicated that the catalyst performance of hydrotalcite-derived NiAl catalysts is superior to Ni/Al2O3 catalysts prepared by the conventional impregnation method, which maybe due to the better Ni dispersion and uniform average particle size distribution with around 12.7 nm compared with the agglomeration of the Ni/Al2O3 particles for up to 53.2 nm. The catalyst with a Ni/Al molar ratio of 3 exhibited the optimal catalytic activity with a stability for 75 min at nearly 90 % hydrogen yield at 700 °C. The reaction temperature also suggested a positive correlation between the hydrogen yield and the reaction temperature from 600 °C to 800 °C. Moreover, based on the investigation of the catalysts during the reaction transition state, Ni particles sintered rapidly from 10.2 nm to 31.2 nm at the beginning reaction time with the high hydrogen yield and then tended to be stable, which may be correlated well with the degree of graphitization of the deposited carbon. This paper provides a valuable design for efficient methane cracking catalysts.