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In Situ Surficial Polymerization of Ultrahigh-Nickel Cathode Material for Stable Solid-State Lithium Batteries
Yuqing Dai1, Zihan Hou1, Xin Yu1
1National Energy Metal Resources and New Materials Key Laboratory, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy, School of Metallurgy and Environment, Central South University, Changsha 410083, China.
ACS Applied Materials & Interfaces
|April 1, 2025
Summary
A novel nanoscale polymer coating effectively protects ultrahigh-nickel cathode active materials (CAMs) in solid-state lithium-metal batteries (SLMBs). This surface modification prevents side reactions with poly(ethylene oxide) (PEO) electrolytes, enhancing battery stability and longevity.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Science
Background:
- Ultrahigh-nickel cathode active materials (CAMs) are crucial for high-energy solid-state lithium-metal batteries (SLMBs).
- These CAMs undergo detrimental side reactions with conventional poly(ethylene oxide) (PEO)-based electrolytes, limiting battery performance and lifespan.
- Developing protective strategies for CAM surfaces is essential for advancing SLMB technology.
Purpose of the Study:
- To develop a surface modification strategy for ultrahigh-nickel CAMs to mitigate side reactions with PEO electrolytes.
- To investigate the mechanism of in situ polymerization and the role of oxygen vacancies in enhancing Li+ transport.
- To evaluate the electrochemical performance and stability of the modified CAMs in SLMBs.
Main Methods:
- A self-assembled nanoscale polymer coating was applied to ultrahigh-nickel CAMs using inherent residual lithium compounds as initiators for in situ anionic polymerization.
- Oxygen vacancies were generated on the CAM surface via coordination of functional groups with transition metal ions.
- Electrochemical performance was assessed using LiNi0.9Co0.06Mn0.04O2 cathodes with PEO-based electrolytes in SLMBs.
- Polymer decomposition was analyzed using gel permeation chromatography (GPC) to measure the molecular weight (Mw) of recycled PEO.
Main Results:
- The nanoscale polymer coating significantly improved the stability of ultrahigh-nickel CAMs against PEO-based electrolytes.
- The coated LiNi0.9Co0.06Mn0.04O2 cathode retained 92% of its capacity after 100 cycles.
- SLMBs utilizing the coated CAMs demonstrated stable operation for 500 cycles at 1C.
- GPC analysis confirmed the inhibition of PEO decomposition, evidenced by the preserved molecular weight of recycled PEO.
Conclusions:
- The proposed surface modification strategy effectively enhances the electrochemical performance and cycle life of SLMBs by protecting ultrahigh-nickel CAMs.
- The nanoscale polymer coating facilitates rapid Li+ transfer and provides elasticity, contributing to improved battery stability.
- This efficient and scalable coating method holds promise for the commercialization of advanced solid-state batteries.
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