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Mechanically Adaptive Cathode-Electrolyte Interphase via Dynamic Covalent Chemistry for Long-Life Ni-Rich Lithium
Yi-Shun Li1, Yao-Lu Ye1, Zi-Xin Xie1
1College of Chemistry, Huazhong Agricultural University, Wuhan 430070, China.
Journal of the American Chemical Society
|September 3, 2025
Summary
Engineered a self-healing cathode coating for high-nickel batteries. This dynamic interface enhances stability and longevity in lithium-ion batteries by accommodating mechanical stress.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- High-nickel cathodes like LiNi0.83Co0.12Mn0.05O2 (NCM83) exhibit interfacial instability.
- Cathode-electrolyte reactions and mechanical strain cause degradation in NCM83 performance.
Purpose of the Study:
- To develop a mechanically adaptive cathode-electrolyte interphase (CEI) for NCM83 cathodes.
- To enhance the stability and cycling performance of high-nickel lithium-ion batteries.
Main Methods:
- Engineered a CEI using a supramolecular ion-conducting polyurethane ureido-pyrimidinone (SPU-UPy) elastomer with dynamic covalent bonds (hydrogen and disulfide).
- Incorporated transition metal ion-O/N coordination bonds for improved adhesion and reduced metal dissolution.
- Utilized a polyether backbone for efficient Li-ion transport.
Main Results:
- The SPU-UPy CEI demonstrated exceptional mechanical resilience and self-healing properties.
- Coated NCM83 cathodes showed enhanced adhesion and suppressed transition metal dissolution.
- Achieved 82.2% capacity retention after 400 cycles at 1 C, indicating superior long-term cycling stability.
Conclusions:
- Dynamic covalent chemistry is crucial for stabilizing Ni-rich cathode interfaces.
- Mechano-adaptive interfacial engineering offers a new strategy for designing high-energy-density batteries.
- The SPU-UPy elastomer presents a promising approach for next-generation battery materials.
