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From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding
Published on: March 24, 2018
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Enhanced inorganic-organic interphase compatibility in composite solid electrolytes by forming isocyanate-linked
Xiaorong Zhang1, Jinping He1, Yuxue Sun1
1National & Local United Engineering Laboratory for Power Battery, Department of Chemistry, Northeast Normal University, Changchun 130024, China.
Journal of Colloid and Interface Science
|July 18, 2025
Summary
Chemically grafting solid electrolytes with isocyanates improves compatibility in solid-state lithium metal batteries. This creates stable interfaces and enhances ionic conductivity for safer, high-energy batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- Solid-state lithium metal batteries (SSLMBs) offer high energy density and safety.
- Composite solid electrolytes (CSEs) face challenges with inorganic-organic phase separation, hindering performance.
- Improving interfacial compatibility is crucial for advanced SSLMBs.
Purpose of the Study:
- To develop a novel organic-inorganic hybrid cross-linked CSE for SSLMBs.
- To enhance the compatibility between inorganic and organic phases in CSEs.
- To improve the ionic conductivity and cycling stability of SSLMBs.
Main Methods:
- Chemical grafting of 2-isocyanatoethyl methacrylate (IEM) onto Li6.4La3Zr1.4Ta0.6O12 (LLZTO) to create LLZTO@IEM.
- Copolymerization of LLZTO@IEM with N,N'-methylenebisacrylamide (MBA) and poly(ethylene glycol methyl ether methacrylate) (PEGMA) under UV illumination.
- Incorporation of succinonitrile (SN) to further enhance interfacial compatibility.
Main Results:
- The resulting CSE (PMIS@LLZTO) exhibited high ionic conductivity (3.36 × 10⁻⁴ S cm⁻¹) and a high lithium-ion transference number (0.73).
- Li/PMIS@LLZTO/Li symmetric cells showed stable cycling for over 3000 hours with minimal polarization.
- Full cells with LiFePO4 and LiNi0.6Mn0.2Co0.2O2 cathodes demonstrated excellent initial capacities and long-term cycling stability.
Conclusions:
- Chemical grafting using isocyanates is a scalable method for designing high-performance CSEs.
- The developed PMIS@LLZTO composite solid electrolyte significantly enhances interfacial compatibility and electrochemical performance in SSLMBs.
- This approach paves the way for safer and more efficient solid-state batteries.
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