Plastic waste has become an alternative resource for generating carbon-free hydrogen and valuable carbon. The challenge lies in the efficient catalytic pyrolysis of plastics, the energy-intensive nature of decomposition, and reactor configuration. In a single-stage process, the presence of solid plastic with the catalyst leads to carbon block formation, inhibiting the growth of filamentous structure. We proposed a two-stage process incorporating microwave-assisted heating, encompassing thermal pyrolysis at 500 ˚C, followed by catalytic chemical vapor deposition at 800 ˚C. Transition metals, including iron, nickel, and cobalt, and their alloys were examined for catalytic performance along with assessments of catalyst-to-feed mixing ratios and catalyst stability. Comprehensive characterization techniques were employed to explore nanocrystal size, dispersion, reduction behavior, and support interaction strength. The FeNi/Al2O3 catalyst exhibited the highest yields among the selected catalysts, attributed to its optimized nanocrystalline size and interaction strength. These characteristics facilitated the production of 445 mg/gplastic of carbon nanotubes and 52.1 mmol/gplastic of hydrogen during low-density polyethylene decomposition, corresponding to the extraction of 52 % carbon and 72 % hydrogen relative to theoretical content. The catalyst exhibited a sustained efficiency over ten consecutive cycles, yielding 513 mg/gplastic of highly crystalline multiwall carbon nanotubes, with electrification demonstrating promise for sustainably converting plastic waste into carbon-free hydrogen and carbon.
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