ABSTRACT Composite polymer electrolytes (CPEs) have attracted worldwide growing attention in the field of lithium‐ion batteries (LIBs), mainly because of their excellent ionic conductivity, improved thermal and electrochemical stability, and enhanced flexibility. In this work, we prepared nanocomposite gel polymer electrolytes (NCGPEs) as advanced functional materials based on poly(methyl methacrylate) (PMMA) and halloysite nanotubes (HNTs), followed by modification with γ‐(trimethoxysilyl)propyl methacrylate (γ‐MPS) and subsequently grafting with PMMA (mHNT‐ g ‐PMMA). The tubular structure of HNTs, along with novel ion transport pathways provided by the developed functional nanostructure significantly improved the ionic conductivity, and charge‐discharge performance. The optimal sample, containing 2 wt. % mHNT‐ g ‐PMMA displays an impressive ionic conductivity measured at 2.4 × 10 −4 S cm −1 , and a t + number of 0.86. Furthermore, it demonstrates an excellent initial discharge capacity of 180 mAh g −1 and remarkable electrochemical stability above 6 V. Notably, it maintains 100% Coulombic efficiency and capacity retention over 100 cycles at 1C, employing high‐voltage FeFe(CN) 6 cathode and graphite anode. FE‐SEM images demonstrate that HNTs effectively suppress dendrites following 100 charge‐discharge cycles under a current density of 1C. Even at a high C‐rate (5C), the system maintains a capacity of 173 mAh g −1 . These results suggest that the newly‐developed NCGPEs are excellent candidates for use in high‐performance LIBs.
Anavi et al. (2026) studied this question.