Impact of nickel and alkaline earth metals interaction on sustainable carbon nanotubes generation from plastic face masks via catalytic pyrolysis

The one-pot synthesis of carbon nanotubes (CNTs) emerges as a promising approach for plastic valorization, owing to its simplicity and scalability. However, limited attention has been given to catalyst design for this method, particularly regarding the influence of Group 2 alkaline earth metal elements (X) on the Ni-based catalyst activity. This study investigates the impact of X on the catalytic activity of Ni towards sustainable CNTs synthesis using plastic face masks. The findings revealed that X influenced the carbon yield of NiMo-X catalysts and the morphology of the resultant carbon nanomaterials. Notably, NiMo-Ca demonstrated the highest carbon yield, whereas NiMo-Mg and NiMo-Ba exhibited the lowest. Furthermore, NiMo-Mg tends to produce clean and thin CNTs, while NiMo-Ba tends to yield carbon flakes with numerous irregular cokes. In addition to the effect of Ni crystallite size, which influences the transition from tubular to flake-like carbon structures, environmental factors are also considered. Specifically, NiMo-Mg generated a high CO₂/CH₄ environment, while NiMo-Ba exhibited slower catalytic cracking of polymeric chains from face masks, both of which were unfavorable for CNTs growth. Conversely, NiMo-Ca facilitated higher carbon recovery, likely due to its creation of a low CO₂/CH₄ environment via CO₂ methanation. Optimization studies indicated that increasing pyrolysis temperatures and durations lead to reduced carbon yield, while cyclic pyrolysis of face masks up to five iterations enhances the reusability of NiMo-X catalysts with improved carbon recovery. Overall, this study provides valuable insights into the early pyrolytic gas formation and carbon nucleation phase, which are influenced by the surface Ni fraction and Ni polarization, as well as the later CNTs growth phase, which is related to the Ni crystallite size.