Methylcyclohexane-assisted polypropylene upcycling over PtRu/Al₂O₃ via tandem dehydrogenation-hydrogenolysis.
- 1Chemistry Research Laboratory, Department of Chemistry, University of Oxford 12 Mansfield Road Oxford OX1 3TA UK [email protected].
- 2Department of Engineering Science, University of Oxford Parks Road Oxford OX1 3PJ UK.
- 3Inorganic Chemistry Laboratory, University of Oxford South Parks Road Oxford OX1 3QR UK.
Abstract
Catalytic hydroconversion of polyolefin waste typically relies on the addition of high-pressure hydrogen, which greatly impacts both the process implementation and economic viability. Here we report polypropylene (PP) hydrogenolysis coupled to methylcyclohexane (MCH) dehydrogenation providing an external-H₂-free tandem route to naphtha-range liquid hydrocarbons. The best performing catalysis system was 1 nm sized PtRu nanoparticles (1 wt% Pt/1 wt% Ru) on γ-Al₂O₃. At 300 °C, this catalyst could facilitate over 96 wt% PP conversion with more than 88 wt% as naphtha-range liquid hydrocarbon products. This performance was retained over 6 recycles. Spectroscopic characterisation indicates the formation of electronically coupled PtRu domains, which promote MCH dehydrogenation and moderate C-C bond cleavage. Solvent screening shows that hydrocarbon liquids with different structures lead to pronounced differences in PP conversion and product selectivity. Molecular dynamics simulations of PP in representative solvents provide a qualitative picture of how solvent-dependent chain mobility and chain extension may influence polymer accessibility to catalytic sites. Techno-economic analysis and life-cycle assessment suggest that, under favorable feedstock assumptions, renewable MCH could lower both carbon intensity and production cost relative to a direct H₂-based route. These results identify MCH-assisted PtRu nanoparticle catalysis as a viable tandem process for PP upcycling and highlight the importance of coupling hydrogen-donor chemistry with liquid-phase transport effects in plastic waste valorisation.
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BibTeX
@article{wang2026methylcyclohexaneassisted,
title = {{Methylcyclohexane-assisted polypropylene upcycling over PtRu/Al₂O₃ via tandem dehydrogenation-hydrogenolysis.}},
author = {Haokun Wang and Zhiyuan Zong and Mingyu Luo and Frederick Z T Yang and Jiaying Pan and Zeyu Wu and Rui Liu and Yuhong Luo and Jiasi Li and Yiyang Li and Roland C Turnell-Ritson and Michail Stamatakis and Aidong Yang and Dermot O' Hare},
journal = {Energy \& environmental science},
year = {2026},
month = oct,
doi = {10.1039/d6ee05130h},
url = {https://europepmc.org/article/MED/42948402},
note = {CC BY},
}
RIS
TY - JOUR
TI - Methylcyclohexane-assisted polypropylene upcycling over PtRu/Al₂O₃ via tandem dehydrogenation-hydrogenolysis.
AU - Haokun Wang
AU - Zhiyuan Zong
AU - Mingyu Luo
AU - Frederick Z T Yang
AU - Jiaying Pan
AU - Zeyu Wu
AU - Rui Liu
AU - Yuhong Luo
AU - Jiasi Li
AU - Yiyang Li
AU - Roland C Turnell-Ritson
AU - Michail Stamatakis
AU - Aidong Yang
AU - Dermot O' Hare
PY - 2026
DA - 2026/10/27
JO - Energy & environmental science
DO - 10.1039/d6ee05130h
UR - https://europepmc.org/article/MED/42948402
AB - Catalytic hydroconversion of polyolefin waste typically relies on the addition of high-pressure hydrogen, which greatly impacts both the process implementation and economic viability. Here we report polypropylene (PP) hydrogenolysis coupled to methylcyclohexane (MCH) dehydrogenation providing an external-H₂-free tandem route to naphtha-range liquid hydrocarbons. The best performing catalysis system was 1 nm sized PtRu nanoparticles (1 wt% Pt/1 wt% Ru) on γ-Al₂O₃. At 300 °C, this catalyst could facilitate over 96 wt% PP conversion with more than 88 wt% as naphtha-range liquid hydrocarbon products. This performance was retained over 6 recycles. Spectroscopic characterisation indicates the formation of electronically coupled PtRu domains, which promote MCH dehydrogenation and moderate C-C bond cleavage. Solvent screening shows that hydrocarbon liquids with different structures lead to pronounced differences in PP conversion and product selectivity. Molecular dynamics simulations of PP in representative solvents provide a qualitative picture of how solvent-dependent chain mobility and chain extension may influence polymer accessibility to catalytic sites. Techno-economic analysis and life-cycle assessment suggest that, under favorable feedstock assumptions, renewable MCH could lower both carbon intensity and production cost relative to a direct H₂-based route. These results identify MCH-assisted PtRu nanoparticle catalysis as a viable tandem process for PP upcycling and highlight the importance of coupling hydrogen-donor chemistry with liquid-phase transport effects in plastic waste valorisation.
SN - 1754-5692
SN - 1754-5706
ER -