Selective electrified polyethylene upcycling by pore-modulated pyrolysis

Yang, Ji [Yale Univ., New Haven, CT (United States); Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000339110816); Dong, Qi [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000275534213); Zhang, Chunyan [Univ. of Delaware, Newark, DE (United States)] (ORCID:0000000204655181); Zhang, Wentao [Yale Univ., New Haven, CT (United States)] (ORCID:0009000378286096); Miscall, Joel [National Renewable Energy Laboratory (NREL), Golden, CO (United States)]; Brozena, Alexandra H. [Yale Univ., New Haven, CT (United States)]; Chen, Jiansong [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000320462352); Liu, Ning [Princeton Univ., NJ (United States)] (ORCID:0000000190799351); Li, Tangyuan [Yale Univ., New Haven, CT (United States)] (ORCID:0009000112320613); Liu, Fangyuan [Yale Univ., New Haven, CT (United States)]; Nascimento, Claudemi A. [West Virginia Univ., Morgantown, WV (United States)]; Dantas, Beatriz [West Virginia Univ., Morgantown, WV (United States)]; Zhang, Bohong [Missouri Univ. of Science and Technology, Rolla, MO (United States)] (ORCID:0000000255748396); Mumtaz, Farhan [Missouri Univ. of Science and Technology, Rolla, MO (United States)]; Liu, Zixiao [Univ. of Delaware, Newark, DE (United States)]; Liu, Shufeng [Yale Univ., New Haven, CT (United States)]; Du, Yiheng [Yale Univ., New Haven, CT (United States)]; Wang, Ziyu [Princeton Univ., NJ (United States)] (ORCID:0000000329146460); Pang, Zhiqiang [Univ. of Wisconsin, Madison, WI (United States)]; Liu, Dongxia [Univ. of Delaware, Newark, DE (United States)]; Huang, Jie [Missouri Univ. of Science and Technology, Rolla, MO (United States)] (ORCID:0000000286592910); Lima, Fernando V. [West Virginia Univ., Morgantown, WV (United States)] (ORCID:0000000343061826); Pan, Xuejun [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000268599342); Ju, Yiguang [Princeton Univ., NJ (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)] (ORCID:0000000256562075); Fu, Kelvin [Univ. of Delaware, Newark, DE (United States)] (ORCID:000000034963615X); Hu, Shu [Yale Univ., New Haven, CT (United States)] (ORCID:0000000250410169); Beckham, Gregg T. [National Renewable Energy Laboratory (NREL), Golden, CO (United States)] (ORCID:000000023480212X); Hu, Liangbing [Yale Univ., New Haven, CT (United States); Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000294569315)

doi:10.1038/s44286-025-00248-0

DOE OSTI · 3031036

Selective electrified polyethylene upcycling by pore-modulated pyrolysis

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Abstract

Plastic waste is a increasing problem, accumulating in landfills and the environment. Pyrolysis is a promising and industrially relevant approach for transforming plastic waste into value-added chemicals. However, the selectivity and yield of traditional plastic pyrolysis are poor, with products featuring broad molar mass distributions. Here we report a highly selective, energy-efficient and catalyst-free pyrolysis method that can upcycle plastic into value-added chemicals via pore-modulated pyrolysis. Using a Joule-heated carbon column, we demonstrate the pivotal role of the reactor’s graded porous structure in decreasing the polydispersity of the reaction intermediates, enabling high product selectivity and yield. The decreasing pore size of the reactor modulates the mass transport in an apparent gating effect—preventing high-molar-mass species from exiting the reactor before sufficient pyrolysis has occurred. Using polyethylene as a model reactant, we demonstrate a high yield of 65.9 ± 5.2% and up to 80.8% selectivity toward value-added aviation fuel precursor (C8–C18 hydrocarbons) without the use of any catalysts.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY 3D printing electrified pyrolysis mass transport and heat transfer control plastic upcycling pore-regulated reaction

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Yang, Ji [Yale Univ., New Haven, CT (United States); Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000339110816), Dong, Qi [Purdue Univ., West Lafayette, IN (United States)] (ORCID:0000000275534213), Zhang, Chunyan [Univ. of Delaware, Newark, DE (United States)] (ORCID:0000000204655181), Zhang, Wentao [Yale Univ., New Haven, CT (United States)] (ORCID:0009000378286096), Miscall, Joel [National Renewable Energy Laboratory (NREL), Golden, CO (United States)], Brozena, Alexandra H. [Yale Univ., New Haven, CT (United States)], Chen, Jiansong [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000320462352), Liu, Ning [Princeton Univ., NJ (United States)] (ORCID:0000000190799351), Li, Tangyuan [Yale Univ., New Haven, CT (United States)] (ORCID:0009000112320613), Liu, Fangyuan [Yale Univ., New Haven, CT (United States)], Nascimento, Claudemi A. [West Virginia Univ., Morgantown, WV (United States)], Dantas, Beatriz [West Virginia Univ., Morgantown, WV (United States)], Zhang, Bohong [Missouri Univ. of Science and Technology, Rolla, MO (United States)] (ORCID:0000000255748396), Mumtaz, Farhan [Missouri Univ. of Science and Technology, Rolla, MO (United States)], Liu, Zixiao [Univ. of Delaware, Newark, DE (United States)], Liu, Shufeng [Yale Univ., New Haven, CT (United States)], Du, Yiheng [Yale Univ., New Haven, CT (United States)], Wang, Ziyu [Princeton Univ., NJ (United States)] (ORCID:0000000329146460), Pang, Zhiqiang [Univ. of Wisconsin, Madison, WI (United States)], Liu, Dongxia [Univ. of Delaware, Newark, DE (United States)], Huang, Jie [Missouri Univ. of Science and Technology, Rolla, MO (United States)] (ORCID:0000000286592910), Lima, Fernando V. [West Virginia Univ., Morgantown, WV (United States)] (ORCID:0000000343061826), Pan, Xuejun [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000268599342), Ju, Yiguang [Princeton Univ., NJ (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)] (ORCID:0000000256562075), Fu, Kelvin [Univ. of Delaware, Newark, DE (United States)] (ORCID:000000034963615X), Hu, Shu [Yale Univ., New Haven, CT (United States)] (ORCID:0000000250410169), Beckham, Gregg T. [National Renewable Energy Laboratory (NREL), Golden, CO (United States)] (ORCID:000000023480212X), Hu, Liangbing [Yale Univ., New Haven, CT (United States); Univ. of Maryland, College Park, MD (United States)] (ORCID:0000000294569315). 2025-07-22. Selective electrified polyethylene upcycling by pore-modulated pyrolysis. https://doi.org/10.1038/s44286-025-00248-0

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