Synthesis of high-quality graphene sheets via decomposition of non-condensable gases from pyrolysis of polypropylene waste using unsupported Fe, Co, and Fe–Co catalysts

Abstract

Producing high-quality graphene sheets from plastic waste is regarded as a significant economic and environmental challenge. In the present study, unsupported Fe, Co, and Fe–Co oxide catalysts were prepared by the combustion method and examined for the production of graphene via a dual-stage process using polypropylene (PP) waste as a source of carbon. The prepared catalysts and the as-produced graphene sheets were fully characterized by several techniques, including XRD, H2-TPR, FT-IR, FESEM, TEM, and Raman spectroscopy. XRD, TPR, and FT-IR analyses revealed the formation of high purity and crystallinity of Fe2O3 and Co3O4 nanoparticles as well as cobalt ferrite (CoFe2O4) species after calcining Fe, Co, and Fe–Co catalysts, respectively. The Fe–Co catalyst was completely changed into Fe–Co alloy after pre-reduction at 800 °C for 1 h. TEM and XRD results revealed the formation of multi-layered graphene sheets on the surface of all catalysts. Raman spectra of the as-deposited carbon showed the appearance of D, G, and 2D bands at 1350, 1580, and 2700 cm−1, respectively, confirming the formation of graphene sheets. Fe, Co, and Fe–Co catalysts produced quasi-identical graphene yields of 2.8, 3.04, and 2.17 gC/gcat, respectively. The graphene yield in terms of mass PP was found to be 9.3, 10.1, and 7.2 gC/100gPP with the same order of catalysts. Monometallic Fe and Co catalysts produced a mix of small and large-area graphene nanosheets, whereas the bimetallic Fe–Co catalyst yielded exclusively large-area graphene sheets with remarkable quality. The higher stability of Fe–Co alloy and its carbide phase during the growth reaction compared to the Fe and Co catalysts was the primary reason for the generation of extra-large graphene sheets with relatively low yield. In contrast, the segregation of some metallic Fe or Co particles through the growth time was responsible for the growth small-area graphene sheets.