Preparation and growth mechanism of high-quality multilayer graphene from simulated coal pyrolysis gas via chemical vapor deposition

Chemical vapor deposition (CVD) of graphene from coal pyrolysis gas provides new ways for both large-scale graphene preparation and high value-added utilization of coal. However, green, efficient and continuous preparation of high-quality multilayer graphene with both good uniformity and ideal structure characteristic remains a great challenge. Herein, we first investigated the influence of main carbonaceous species (CH₄, C₂H₆, C₃H₈, CO₂, and CO) in coal pyrolysis gas on the quality of CVD graphene products. The experimental results indicated that CO₂ and CO have little effect on the growth of graphene, while methane as carbon source is conducive to obtain ideal graphene materials, propane and ethane could also influence structural defects and layer number of graphene products remarkably. On this basis, we designed a mixed gas of methane, ethane, and propane with optimized ratio as simulated coal pyrolysis gas, and successfully prepared high-quality multilayer graphene products on nickel foam from the as-designed simulated coal pyrolysis gas by CVD method. Notably, with a CH₄:C₂H₆:C₃H₈ ratio of 2:1:1, the graphene products prepared from simulated coal pyrolysis gas outperformed that of raw coal pyrolysis gas in terms of physical structure, layer number, and quality uniformity. The corresponding I_2D/I_G value reached 0.97. The graphene growth process and mechanism were investigated and discussed macroscopically and microscopically. This work is of great significance for the intrinsic understanding of CVD growth of graphene from coal pyrolysis gas, and also inspires an efficient and environmentally friendly avenue for high-throughput, uniform production of high-quality graphene materials.