Tailoring Electric Double Layer by Cation Specific Adsorption for High-Voltage Quasi-Solid-State Lithium Metal...

The interfacial instability of high-nickel layered oxides severely plagues practical application of high-energy quasi-solid-state lithium metal batteries (LMBs). Herein, a uniform and highly oxidation-resistant polymer layer within inner Helmholtz plane is engineered by in situ polymerizing 1-vinyl-3-ethylimidazolium (VEIM) cations preferentially adsorbed on LiNi_0.83Co_0.11Mn_0.06O₂ (NCM83) surface, inducing the formation of anion-derived cathode electrolyte interphase with fast interfacial kinetics. Meanwhile, the copolymerization of [VEIM][BF₄] and vinyl ethylene carbonate (VEC) endows P(VEC-IL) copolymer with the positively-charged imidazolium moieties, providing positive electric fields to facilitate Li⁺ transport and desolvation process. Consequently, the Li||NCM83 cells with a cut-off voltage up to 4.5 V exhibit excellent reversible capacity of 130 mAh g^-1 after 1000 cycles at 25 °C and considerable discharge capacity of 134 mAh g^-1 without capacity decay after 100 cycles at -20 °C. This work provides deep understanding on tailoring electric double layer by cation specific adsorption for high-voltage quasi-solid-state LMBs.