Plastic upgrading via catalytic pyrolysis with combined metal-modified gallium-based HZSM-5 and MCM-41

Abstract

Currently, the conversion of waste plastics into high-value products via catalytic pyrolysis enables the advancement of plastics’ open-loop recycling. However, enhancing selectivity remains a critical challenge. This study introduces a novel approach to catalytic pyrolysis, utilizing a combination of MCM-41 and modified gallium-based HZSM-5 catalysts, to achieve exceptional selectivity for aromatic liquid-phase products from linear low-density polyethylene. Firstly, to enhance the probability of dehydroaromatization optimization, the type and proportion of metal active sites within the HZSM-5 catalyst are fine-tuned, which would establish equilibrium with acid sites, resulting in a remarkable 15.72% increase in the selectivity of aromatic hydrocarbons. Secondly, to enhance the accessibility of volatiles to active sites, mesoporous MCM-41 with cracking capabilities is introduced. The doping ratio of MCM-41 is meticulously controlled to facilitate the diffusion of cracked volatiles to the active centers of modified gallium-based HZSM-5, enabling efficient reforming reactions. Experimental findings demonstrate that MCM-41 significantly enhances the dehydroaromatization activity of the modified gallium-based HZSM-5 catalyst. Under the influence of MCM-41:Zr₂Ga₃/HZSM-5 = 1:2 catalyst, the selectivity for aromatic hydrocarbons reaches an impressive 93.11%, with a notable 60.01% selectivity for benzene, toluene, ethylbenzene, and xylene. Lastly, this study proposes a plausible pathway for the generation of high-value aromatic hydrocarbons using the combined catalyst.

Keywords

polyethylene pyrolysis / aromatic hydrocarbons / bimetal catalyst / HZSM-5 / MCM-41

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Competing interests

The authors declare that they have no competing interests.

Acknowledgements

The work was supported by the National Natural Science Foundation of China (Grant No. 22078278); Hunan Innovative Talent Project (Grant No. 2022RC1111); the Key Project of Hunan Provincial Education Department (Grant No. 22A0131).

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