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Abstract 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 0.83 Co 0.11 Mn 0.06 O 2 (NCM83) surface, inducing the formation of anion‐derived cathode electrolyte interphase with fast interfacial kinetics. Meanwhile, the copolymerization of VEIMBF 4 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.
Zhou et al. (Mon,) studied this question.