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PreprintCC BY-NC-NDChemRxiv

Fluorine-Free Gas Diffusion Media for Polymer Electrolyte Fuel Cells Part I: Silicone-based Microporous Layers

  1. 1Chemical Engineering and Chemistry , Eindhoven University of Technology, Het Kranenveld 14, Eindhoven, North Brabant , Netherlands, 5600MB

Abstract

The widespread use of fluoropolymers in electrochemical energy systems, coupled with increasing environmental, health, and regulatory concerns surrounding per- and polyfluoroalkyl substances (PFAS), is motivating the development of fluorine-free alternatives. Here, silicone-based resins are evaluated as fluorine-free binders for microporous layers (MPLs) and integrated into fully fluorine-free gas diffusion media (GDMs). Using Sylgard 184 silicone elastomer, the binder content was systematically varied, identifying 25 wt.% as the lowest loading that provided sufficient water repellency. At this loading, the influence of binder chemistry was investigated by replacing Sylgard 184 with KR-220L, a methyl silicone rigid resin. Although the resin chemistry strongly affected MPL thickness, porosity, and crack formation, its impact on fuel-cell performance was limited. Fully fluorinefree GDMs were then fabricated by depositing silicone-based MPLs onto carbon fiber substrates hydrophobized via organosilicon electrografting. Replacing a commercial PTFEtreated substrate with the fluorine-free electrografted substrate resulted in only a minor decrease in current density, from 4.2 to 4.0 A cm-2 at 0.3 V under high-humidity conditions; both exceeded the commercial fluorinated reference (3.8 A cm-2). Accelerated stress testing further demonstrated promising durability. Overall, silicone-based materials represent a viable route toward replacing fluorinated components in GDMs.

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BibTeX
@misc{sinisgalli2026fluorinefree,
  title = {{Fluorine-Free Gas Diffusion Media for Polymer Electrolyte Fuel Cells Part I: Silicone-based Microporous Layers}},
  author = {Irene Sinisgalli and Nicolaas J. M. van Leth and Antoni Forner-Cuenca},
  howpublished = {ChemRxiv},
  year = {2026},
  month = aug,
  doi = {10.26434/chemrxiv.15008053/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008053/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Fluorine-Free Gas Diffusion Media for Polymer Electrolyte Fuel Cells Part I: Silicone-based Microporous Layers
AU  - Irene Sinisgalli
AU  - Nicolaas J. M. van Leth
AU  - Antoni Forner-Cuenca
PY  - 2026
DA  - 2026/08/30
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008053/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008053/v1
AB  - The widespread use of fluoropolymers in electrochemical energy systems, coupled with increasing environmental, health, and regulatory concerns surrounding per- and polyfluoroalkyl substances (PFAS), is motivating the development of fluorine-free alternatives. Here, silicone-based resins are evaluated as fluorine-free binders for microporous layers (MPLs) and integrated into fully fluorine-free gas diffusion media (GDMs). Using Sylgard 184 silicone elastomer, the binder content was systematically varied, identifying 25 wt.% as the lowest loading that provided sufficient water repellency. At this loading, the influence of binder chemistry was investigated by replacing Sylgard 184 with KR-220L, a methyl silicone rigid resin. Although the resin chemistry strongly affected MPL thickness, porosity, and crack formation, its impact on fuel-cell performance was limited. Fully fluorinefree GDMs were then fabricated by depositing silicone-based MPLs onto carbon fiber substrates hydrophobized via organosilicon electrografting. Replacing a commercial PTFEtreated substrate with the fluorine-free electrografted substrate resulted in only a minor decrease in current density, from 4.2 to 4.0 A cm-2 at 0.3 V under high-humidity conditions; both exceeded the commercial fluorinated reference (3.8 A cm-2). Accelerated stress testing further demonstrated promising durability. Overall, silicone-based materials represent a viable route toward replacing fluorinated components in GDMs.
ER  -