Abstract
Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) has broad applications across various metal-ion battery systems, such as a binder for electrodes, a supporting matrix for electrolytes, and a separator material. Due to its excellent mechanical properties, PVDF-HFP has become an excellent candidate for fabricating gel and solid-state electrolytes in sodium-based batteries. However, in this study, we noticed notable side reactions occurring at the interface of PVDF-HFP membranes and Na metal. These reactions not only alter chemical compositions but also further affect the surface morphology and adhesive properties of membranes. Similar phenomena are observed in other polyfluoroalkyl-based membranes (PVDF and PTFE). Therefore, we systematically studied the reaction mechanisms between the Na metal and these polymers. The influence of different functional groups (−F, −CF3, −H) and their arrangement on the reaction extent has also been discussed. Finally, we concluded with the key factors driving these side reactions and provided new perspectives for designing polymers tailored for sodium-based batteries.
| Original language | English |
|---|---|
| Pages (from-to) | 3513-3520 |
| Number of pages | 8 |
| Journal | JACS Au |
| Volume | 5 |
| Issue number | 7 |
| DOIs | |
| State | Published - Jul 28 2025 |
Funding
This material is based upon work supported by the U.S. Department of Energy, Office of Electricity (OE), Energy Storage Division. Part of this work was authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This work was performed in part at the Georgia Tech Institute for Matter and Systems, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by the National Science Foundation (ECCS-2025462). We thank Lei Cheng and Vaidyanathan Sethuraman for providing the resources and support on the computation study. All authors also want to acknowledge that the computational study was performed using computational resources sponsored by the Department of Energy’s Office of Energy Efficiency and Renewable Energy and located at the National Renewable Energy Laboratory.
Keywords
- Interfacial side reactions
- Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)
- Polytetrafluoroethylene (PTFE)
- Polyvinylidene fluoride (PVDF)
- Sodium (Na)-based battery