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Updated: Jul 3, 2025
Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
Published on: August 12, 2013
Alternatives to fluorinated binders: recyclable copolyester/carbonate electrolytes for high-capacity solid composite
Holly Yeo1, Georgina L Gregory1, Hui Gao1,2,3
1Department of Chemistry, University of Oxford, Chemistry Research Laboratory 12 Mansfield Road Oxford OX1 3TA UK charlotte.williams@chem.ox.ac.uk.
New polymer binders enhance solid-state battery cathodes by improving performance and enabling recycling. These block-copolymers offer high voltage stability and ionic conductivity for next-generation energy storage.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- Optimizing composite cathodes is crucial for commercializing safe, next-generation solid-state batteries.
- Developing suitable polymer binders is essential for electrode processability and stable solid-solid interfaces.
- Traditional binders often limit the performance and recyclability of solid-state battery components.
Purpose of the Study:
- To design and systematically investigate block-polyester/carbonates as Li-ion conducting, high-voltage stable binders for solid-state battery cathodes.
- To compare ABA- and AB-polymeric architectures for their suitability in binder applications.
- To identify optimal polymer characteristics for improved electrochemical performance and interfacial stability.
Main Methods:
- Synthesis of block-polyester/carbonates via catalyzed switching between CO2/epoxide and cyclic monomer ring-opening polymerization.
- Fabrication of composite cathodes using single-crystal LiNi0.8Mn0.1Co0.1O2, Li6PS5Cl solid electrolyte, and carbon nanofibres with the new binders.
- Electrochemical testing (discharge capacity, cycling stability) and characterization of binder properties (ionic conductivity, oxidative stability, viscoelasticity).
Main Results:
- Achieved improved discharge capacities (186 mA h g-1) and capacity retention (96.7% over 200 cycles) compared to traditional binders.
- Demonstrated that ABA-type polymer architectures offer superior conductivity and mechanical properties for binder applications.
- Identified optimal binder properties: molar mass of 50 kg mol-1, 35 wt% polycarbonate, 5.2 V oxidative stability, and 2.2 × 10-4 S cm-1 ionic conductivity.
Conclusions:
- Block-polyester/carbonates are effective binders for high-performance solid-state battery cathodes, enhancing electrochemical performance and interfacial stability.
- Controlled polymerization strategies enable tailoring binder properties for demanding applications with high-voltage cathodes and sulfide electrolytes.
- The developed binders facilitate binder separation and complete recycling, contributing to sustainable battery technology.
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