<p>Plastic waste is a growing 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 (C<sub>8</sub>–C<sub>18</sub> hydrocarbons) without the use of any catalysts.</p><p></p>

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Selective electrified polyethylene upcycling by pore-modulated pyrolysis

  • Ji Yang,
  • Qi Dong,
  • Chunyan Zhang,
  • Wentao Zhang,
  • Joel Miscall,
  • Alexandra H. Brozena,
  • Jiansong Chen,
  • Ning Liu,
  • Tangyuan Li,
  • Fangyuan Liu,
  • Claudemi A. Nascimento,
  • Beatriz Dantas,
  • Bohong Zhang,
  • Farhan Mumtaz,
  • Zixiao Liu,
  • Shufeng Liu,
  • Yiheng Du,
  • Ziyu Wang,
  • Zhiqiang Pang,
  • Dongxia Liu,
  • Jie Huang,
  • Fernando V. Lima,
  • Xuejun Pan,
  • Yiguang Ju,
  • Kelvin Fu,
  • Shu Hu,
  • Gregg T. Beckham,
  • Liangbing Hu

摘要

Plastic waste is a growing 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.