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In Situ-Constructed Elastomeric Interphase for Grain Boundary Stabilization in High-Voltage Layered Oxide Cathodes.
Fan Lin1, Haoqi Fan1, Ziyun Wang1
1Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, Hubei University, Wuhan, Hubei, China.
Advanced Materials (Deerfield Beach, Fla.)
|July 11, 2026
Summary
A novel poly(urea-siloxane) coating stabilizes high-energy layered oxide cathodes by preventing degradation at grain boundaries. This enhances battery performance and longevity for advanced lithium-ion applications.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- Layered oxide cathodes are crucial for high-energy-density lithium-ion batteries.
- Their long-term stability is limited by grain boundary degradation due to chemical corrosion and mechanical stress at high voltages.
Purpose of the Study:
- To develop a stable and elastic coating for layered oxide cathodes.
- To improve the interfacial stability and electrochemical performance of high-voltage cathode materials.
Main Methods:
- In situ polymerization of amine-terminated polydimethylsiloxane and toluene diisocyanate (TDI) to create a poly(urea-siloxane) (PUSi) coating.
- Application of the PUSi coating as a conformal artificial interphase on layered oxide cathode materials (e.g., LiNi0.6Co0.2Mn0.2O2).
Main Results:
- The PUSi coating effectively stabilized cathode interfaces, acting as a chemical barrier against electrolyte reactions and preventing phase transformations.
- The elastic PUSi layer accommodated volume changes, suppressing intergranular cracking during cycling.
- LiNi0.6Co0.2Mn0.2O2 cathodes with PUSi coating retained 81.2% capacity after 450 cycles (coin cells) and 82.4% after 200 cycles (pouch cells) at 4.5 V.
Conclusions:
- The developed PUSi coating offers a scalable and eco-friendly strategy for enhancing the stability and cycle life of high-energy layered oxide cathodes.
- This approach is generalizable to other cathode chemistries, including LiNi0.8Co0.1Mn0.1O2 and lithium-rich layered oxides.
