TY  - JOUR
AU  - Lin, Shenghao
AU  - Cui, Yin
AU  - Yu, Guofang
AU  - Miao, Dongtian
AU  - Liu, Ruliang
AU  - Wu, Dingcai
PY  - 2026
TI  - Asymmetric quasi-solid-state composite electrolytes via self-assembly of molecular brushes and hairy nanoparticles for dendrite-free lithium metal batteries
JO  - Energy Materials and Devices
SN  - 3005-3315
SP  - 9370095
VL  - 4
IS  - 2
AB  - The practical application of lithium metal batteries is severely hindered by flammable liquid electrolytes and uncontrollable lithium dendrite growth. In this study, we propose a novel asymmetric quasi-solid-state composite electrolyte (denoted as QSCE-BPL/LPE/PDL) designed to overcome these challenges. QSCE-BPL/LPE/PDL is fabricated by evaporation-induced self-assembly of one-dimensional molecular brush BC-g-PLiSTFSI [BC = bacterial cellulose, PLiSTFSI = poly(lithium 4-styrenesulfonyl-(trifluoromethylsulfonyl) imide)] and zero-dimensional hairy nanoparticle LL-g-PEGMA [LL = Li6.4La3Zr1.4Ta0.6O12, PEGMA = poly(oligo(ethylene glycol) methyl ether methacrylate)], followed by in situ cationic ring-opening polymerization of 1,3-dioxolane. The resulting ultrathin QSCE-BPL/LPE/PDL (19 μm) possesses a unique asymmetric architecture comprising a rigid layer of hairy nanoparticles to suppress dendrite penetration and a composite layer to ensure good interfacial contact with the cathode. The grafted PLiSTFSI side chains enable single Li+ conduction to reduce concentration polarization, and the PEGMA side chains promote lithium salt dissociation to accelerate Li+ transport. This design yields a three-dimensional porous network that provides continuous and fast Li+ transport pathways. The optimized electrolyte achieves a high ionic conductivity of 5.44 × 10−4 S cm−1 and a Li+ transference number of 0.67 at room temperature. Consequently, Li/LiFePO4 cells with QSCE-BPL/LPE/PDL can operate stably for 200 cycles with a high-capacity retention of 94% at 0.5 C. This study provides a feasible molecular engineering strategy for developing high-performance and safe lithium metal batteries.
UR  - https://doi.org/10.26599/EMD.2026.9370095
DO  - 10.26599/EMD.2026.9370095