Valorizing non-condensable pyrolysis gases from mixed plastic waste: A comprehensive parametric study of the cross-metathesis reaction for propylene production

This work focuses on the valorization of the non-condensable pyrolysis gases (NCPGs) derived from mixed plastic waste (MPW). A feedstock consisting of ethylene and 1-butene, primary constituents of NCPGs, was utilized for propylene production via cross-metathesis reaction. A comprehensive parametric study was performed on a series of xWO 3 /Al-MCM-41 catalysts. The effect of temperature, Si/Al ratio, WO 3 loading, residence time (W cat /F 0 ), feed ratio (ethylene/1-butene), and reactants partial pressure were investigated. Ex situ and in situ characterization techniques (XRD, Raman spectroscopy, TEM, BET, FT-IR (study of pyridine adsorption), TPO, TPR, and EXAFS) were applied to the fresh and used catalysts. Αluminum (Al) incorporation into the MCM-41 structure promoted both Lewis and Brønsted acidity, favoring the isomerization reaction of 1-butene to 2-butene. The tungsten oxo (W=O) species served as the precursor for the active site for propylene production through the cross-metathesis reaction. The 20 wt% WO 3 /Al-MCM-41 catalyst, with a Si/Al ratio of 30, attained a remarkable performance at 550 °C, 1 bar, W cat /F 0 = 117.4 kg Cat ·s·mol −1 and ethylene/1-butene = 4.5/1. Under these conditions, the ethylene and 1-butene conversions reached 28% and 97%, respectively, along with a C-based selectivity of 73% towards propylene. • Non-condensable pyrolysis gases (NCPGs) are a highly valuable output stream. • The catalytic metathesis of ethylene and 1-butene for propylene production was studied. • Incorporating Al into MCM-41 enhances acidity, key for the isomerization of 1-butene. • Excess ethylene/1-butene and longer residence time improved propylene selectivity. • The 20%WO 3 /Al-MCM-41(30) catalyst reached 73% propylene selectivity and 97% 1-butene conversion.

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Journal
Chemical Engineering Journal
Published
2025-06-24
DOI
https://doi.org/10.1016/j.cej.2025.165300
Primary Topic
Catalysis and Hydrodesulfurization Studies
Type
article
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article

Valorizing non-condensable pyrolysis gases from mixed plastic waste: A comprehensive parametric study of the cross-metathesis reaction for propylene production

Stavros Alexandros Theofanidis, Alessandro Longo, Christoph J. Sahle, Dirk E De Vos et al.
Chemical Engineering Journal
Catalysis and Hydrodesulfurization Studies
article

Valorizing non-condensable pyrolysis gases from mixed plastic waste: A comprehensive parametric study of the cross-metathesis reaction for propylene production

Stavros Alexandros Theofanidis, Alessandro Longo, Christoph J. Sahle, Dirk E De Vos, Stamatia A. Karakoulia, Angeliki A. Lemonidou, Ehsan Mahmoudi
article en

Abstract

This work focuses on the valorization of the non-condensable pyrolysis gases (NCPGs) derived from mixed plastic waste (MPW). A feedstock consisting of ethylene and 1-butene, primary constituents of NCPGs, was utilized for propylene production via cross-metathesis reaction. A comprehensive parametric study was performed on a series of xWO 3 /Al-MCM-41 catalysts. The effect of temperature, Si/Al ratio, WO 3 loading, residence time (W cat /F 0 ), feed ratio (ethylene/1-butene), and reactants partial pressure were investigated. Ex situ and in situ characterization techniques (XRD, Raman spectroscopy, TEM, BET, FT-IR (study of pyridine adsorption), TPO, TPR, and EXAFS) were applied to the fresh and used catalysts. Αluminum (Al) incorporation into the MCM-41 structure promoted both Lewis and Brønsted acidity, favoring the isomerization reaction of 1-butene to 2-butene. The tungsten oxo (W=O) species served as the precursor for the active site for propylene production through the cross-metathesis reaction. The 20 wt% WO 3 /Al-MCM-41 catalyst, with a Si/Al ratio of 30, attained a remarkable performance at 550 °C, 1 bar, W cat /F 0 = 117.4 kg Cat ·s·mol −1 and ethylene/1-butene = 4.5/1. Under these conditions, the ethylene and 1-butene conversions reached 28% and 97%, respectively, along with a C-based selectivity of 73% towards propylene. • Non-condensable pyrolysis gases (NCPGs) are a highly valuable output stream. • The catalytic metathesis of ethylene and 1-butene for propylene production was studied. • Incorporating Al into MCM-41 enhances acidity, key for the isomerization of 1-butene. • Excess ethylene/1-butene and longer residence time improved propylene selectivity. • The 20%WO 3 /Al-MCM-41(30) catalyst reached 73% propylene selectivity and 97% 1-butene conversion.

Chemical Engineering JournalVol. 519
Aristotle University of Thessaloniki (GR), European Synchrotron Radiation Facility (FR), Centre for Research and Technology Hellas (GR), KU Leuven (BE)
Horizon 2020 Framework Programme, H2020 Marie Skłodowska-Curie Actions, HORIZON EUROPE Marie Sklodowska-Curie Actions
Responsible consumption and production
Openalex Percentile: Top 86%
Catalysis and Hydrodesulfurization Studies
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