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Updated: Sep 14, 2025
From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding
Published on: March 24, 2018
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.
Abstract:
Solid-state lithium metal batteries (SSLMBs) employing composite solid electrolytes (CSEs) hold immense potential due to their high energy density and enhanced safety. However, the poor compatibility between inorganic and organic phases in CSEs often leads to phase separation, impeding ionic migration and mechanical stability. In this work, we demonstrate for the first time that 2-isocyanatoethyl methacrylate (IEM) can be chemically grafted onto Li6.4La3Zr1.4Ta0.6O12 (LLZTO) via the reaction of isocyanate groups with hydroxyl groups on the surface of LLZTO, yielding modified LLZTO (LLZTO@IEM). Subsequently, LLZTO@IEM is copolymerized with N,N'-methylenebisacrylamide (MBA) and poly(ethylene glycol methyl ether methacrylate) (PEGMA) under ultraviolet (UV) illumination to obtain an organic-inorganic hybrid cross-linked CSE (PMIS@LLZTO) with succinonitrile (SN). Covalently linking LLZTO and the polymer matrix enhances organic-inorganic interphase compatibility and ensures LLZTO to be uniformly dispersed in PMIS@LLZTO, while SN further enhances the interfacial compatibility through coordination with the metal ions on LLZTO surface and reduces the crystallinity of the polymer matrix. PMIS@LLZTO exhibits high ionic conductivity of 3.36 × 10-4 S cm-1 and lithium-ion transference number of tLi+ = 0.73 at 30 °C. Li/PMIS@LLZTO/Li symmetric cell demonstrates stable cycling for over 3000 h with minimal polarization, attributed to robust interfacial compatibility and an inorganic-rich stable solid electrolyte interphase (SEI). Full cells paired with LiFePO4 (LFP) and LiNi0.6Mn0.2Co0.2O2 (NCM622) cathodes deliver high initial capacities (160 and 144 mAh g-1, respectively) and retain 93.8 % and 80 % capacity after 600 and 200 cycles, underscoring exceptional cycling stability. This study demonstrates that chemical grafting of garnet-type fast ionic conductors with isocyanates provides a scalable route to the design of high-performance CSEs.
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