CO2-mediated catalytic upcycling of plastic waste for H2-rich syngas and carbon nanomaterials

To establish a reliable disposal platform of plastic waste, this work developed a novel dual-stage CO2-medaited decomposition-catalysis route by applying multi-functional zeolite-supported bimetallic catalysts. Catalytic upcycling of plastic was first performed in Ar as a reference environment. Bimetallic Fe-Co/ZSM5 catalyst achieved the highest gas yield (53.98 mmol/g), with a H2 proportion of 62.17 vol%. It was evidenced that the Fe-Co alloy had an apparent positive synergistic effect on catalytic cracking and reforming of intermediate volatiles into H2-rich fuel gas and pure carbon nanotubes (CNTs). Regarding CO2-mediated decomposition-catalysis of plastic, there was an apparent synergistic effect between metallic Ni and Fe on gas production so that bimetallic Ni-Fe catalyst gained the maximum cumulative gas yield of 82.33 mmol/g, with a syngas purity of ∼74%. Ni-Fe/ZSM5 also achieved the maximum hydrogen efficiency (87.38%) and CO2-to-CO conversion efficiency (98.62%), implying hydrogen content in plastic and oxygen content in CO2 were essentially converted into gases. Additionally, bimetallic Ni-Fe catalyst revealed the highest carbon production (33.74 wt%), witnessing a synergistic enhancement of 43.45%; specially, approximately 257 mg/g CNTs were anchored on Ni-Fe/ZSM5, with a CNTs purity of over 76%. Overall, this study offers a superb solution in plastic waste valorization and greenhouse gas emission management.