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

doi:10.1007/s11705-024-2476-3

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (11) : 125 https://doi.org/10.1007/s11705-024-2476-3

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

Huaping Lin¹, Likai Zhu¹, Ye Liu¹, Vasilevich Sergey Vladimirovich², Bilainu Oboirien³, Yefeng Zhou¹(

)

¹. National & Local United Engineering Research Centre for Chemical Process Simulation and Intensification, College of Chemical Engineering, Xiangtan University, Xiangtan 411105, China
². Institute of Power Engineering, National Academy of Sciences of Belarus, Minsk 220072, Belarus
³. Department of Chemical Engineering, University of Johannesburg, Johannesburg 17011, South Africa

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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

Corresponding Author(s): Yefeng Zhou

Just Accepted Date: 21 May 2024 Issue Date: 18 July 2024

Cite this article:

Huaping Lin,Likai Zhu,Ye Liu, et al. Plastic upgrading via catalytic pyrolysis with combined metal-modified gallium-based HZSM-5 and MCM-41[J]. Front. Chem. Sci. Eng., 2024, 18(11): 125.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2476-3
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I11/125

Fig.1 Schematic diagram of plastic catalytic pyrolysis experimental setup.

Tab.1 Analysis and instruments

Fig.2 Rapid catalytic pyrolysis products of LLDPE with different metal species combinations. (a) Three-phase product yield distribution, (b) liquid-phase product distribution, and (c) gas-phase product distribution.

Fig.3 Rapid catalytic pyrolysis products of LLDPE at different metal loading levels, including (a) distribution of three-phase yields, (b) distribution of liquid-phase products, and (c) distribution of gas-phase products.

Fig.4 XRD spectra of the parent and metal-modified HZSM-5 zeolites.

Fig.5 SEM images of the parent (a) and Zr₂Ga₃/HZSM-5 (b), along with elemental mapping images (Si, O, Al, Zr, and Ga) for Zr₂Ga₃/HZSM-5 (c).

Tab.2 Surface area, pore volume, and average pore size distribution of the parent and different metal species combination modified HZSM-5 catalysts

Fig.6 Characterization of parent and various metal-modified HZSM-5 catalysts. (a) N₂ adsorption-desorption isotherms, and (b) pore size distribution.

Tab.3 Quantity of acidic sites of parent and metal-modified HZSM-5

Fig.7 NH₃-TPD spectra of the parent and metal-modified HZSM-5.

Fig.8 XPS spectra under different metal loadings. (a) Full spectrum, (b) Zr 3d spectrum, (c) and (d) Ga 3d spectra before and after Ga incorporation.

Tab.4 Selectivity of BTEX in the liquid-phase products obtained from rapid catalytic pyrolysis of LLDPE at different ratios of MCM-41 to Zr₂Ga₃/HZSM-5

Fig.9 Rapid catalytic pyrolysis products of LLDPE at different ratios of MCM-41 to Zr₂Ga₃/HZSM-5. (a) Three-phase product yields, (b) liquid-phase product distribution, and (c) gas-phase product distribution.

Tab.5 Effects of metal load and that after adding MCM-41 in terms of oil yield, selectivity to MAHs and AHs

Tab.6 Evaluation and comparison of different catalysts employed in the open-loop recycling of waste plastics into high-value-added products

Fig.10 Proposed reaction pathway for the rapid catalytic pyrolysis of LLDPE using a mixed catalyst of MCM-41 and Zr₂Ga₃/HZSM-5.

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