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Carbon species deposition is recognized as the primary cause of catalyst deactivation for hydrocarbon cracking and reforming reactions. Exploring the formation mechanism and influencing factors for carbon deposits is crucial for the design of rational catalysts. In this work, a series of NixMgyAl-800 catalysts with nickel particles of varying mean sizes between 13.2 and 25.4 nm were obtained by co-precipitation method. These catalysts showed different deactivation behaviors in the catalytic decomposition of methane (CDM) reaction and the deactivation rate of catalysts increased with the decrease in nickel particle size. Employing TG-MS and TEM characterizations, we found that carbon nanotubes which could keep catalyst activity were more prone to form on large nickel particles, while encapsulated carbon species that led to deactivation were inclined to deposit on small particles. Supported by DFT calculations, we proposed the insufficient supply of carbon atoms and rapid nucleation of carbon precursors caused by the lesser terrace/step ratio on smaller nickel particles, compared with large particles, inhibit the formation of carbon nanotube, leading to the formation of encapsulated carbon species. The findings in this work may provide guidance for the rational design of nickel-based catalysts for CDM and other methane conversion reactions.

Revealing the Effect of Nickel Particle Size on Carbon Formation Type in the Methane Decomposition Reaction