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PreprintCC BY-NC-NDChemRxiv

Controlling polyethylene fibrillation in PFAS-free dry electrodes for processability and electrochemical performance

  • Guillaume Matthews1,2
  • Benjamin Meyer1,2
  • Noël Hallemans3
  • Wenjia Du2,3
  • Paul Shearing2,3
  • Patrick S. Grant1,2
  1. 1Department of Materials, University of Oxford, Parks Road, Oxford, UK, OX1 3PH
  2. 2Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, UK
  3. 3Department of Engineering Science, University of Oxford, Parks Road, Oxford, UK, OX1 3PJ
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Abstract

Ultra-high-molecular-weight polyethylene (UHMWPE) is a more sustainable binder alternative to polytetrafluoroethylene (PTFE) for producing PFAS-free Li-ion battery electrodes using a solvent-free PE fibrillation process. We show that PE fibrillation is thermo-activated and can be controlled to produce an extensive network of nano-fibrils with a median size of 20-40 nm. PE-containing graphite electrode ultimate tensile strength (UTS), critical for roll-to-roll processing, improved more than 20-fold when the electrode calendering temperature increased from 100 to 160-200 °C, providing mechanical stability superior to equivalent PTFE-containing electrodes. PE-containing electrodes calendered at lower temperatures (120-140 °C) showed comparable charging rate performance but superior capacity retention of ∼90% after 100 cycles when compared with PTFE-containing electrodes. Removing PTFE by calcination to mimic direct recycling required temperatures > 600 °C and led to PFAS emissions. In contrast, PE removal was PFAS-free and achieved at 300-400 °C, aided by the catalytic effect of graphite on PE decomposition making PE-containing electrodes more suitable with direct recycling. Overall, integrating across fabrication, mechanical, electrochemical and end-of-life considerations, PE-containing electrodes offer significant potential for more sustainable solvent-free Li-ion batteries.

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Cite

BibTeXRIS
BibTeX
@misc{matthews2026controlling,
  title = {{Controlling polyethylene fibrillation in PFAS-free dry electrodes for processability and electrochemical performance}},
  author = {Guillaume Matthews and Benjamin Meyer and Noël Hallemans and Wenjia Du and Paul Shearing and Patrick S. Grant},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15009336/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009336/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Controlling polyethylene fibrillation in PFAS-free dry electrodes for processability and electrochemical performance
AU  - Guillaume Matthews
AU  - Benjamin Meyer
AU  - Noël Hallemans
AU  - Wenjia Du
AU  - Paul Shearing
AU  - Patrick S. Grant
PY  - 2026
DA  - 2026/09/23
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009336/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009336/v1
AB  - Ultra-high-molecular-weight polyethylene (UHMWPE) is a more sustainable binder alternative to polytetrafluoroethylene (PTFE) for producing PFAS-free Li-ion battery electrodes using a solvent-free PE fibrillation process. We show that PE fibrillation is thermo-activated and can be controlled to produce an extensive network of nano-fibrils with a median size of 20-40 nm. PE-containing graphite electrode ultimate tensile strength (UTS), critical for roll-to-roll processing, improved more than 20-fold when the electrode calendering temperature increased from 100 to 160-200 °C, providing mechanical stability superior to equivalent PTFE-containing electrodes. PE-containing electrodes calendered at lower temperatures (120-140 °C) showed comparable charging rate performance but superior capacity retention of ∼90% after 100 cycles when compared with PTFE-containing electrodes. Removing PTFE by calcination to mimic direct recycling required temperatures > 600 °C and led to PFAS emissions. In contrast, PE removal was PFAS-free and achieved at 300-400 °C, aided by the catalytic effect of graphite on PE decomposition making PE-containing electrodes more suitable with direct recycling. Overall, integrating across fabrication, mechanical, electrochemical and end-of-life considerations, PE-containing electrodes offer significant potential for more sustainable solvent-free Li-ion batteries.
ER  -