Abstract
In-situ fabricated gel polymer electrolytes (GPEs), characterized with superior interfacial properties and large-scale processibility, represent a promising electrolyte system for high-performance lithium metal batteries (LMBs). Herein, we propose an in-situ fabricated high-voltage GPE featuring a localized high-concentration solvation structure (LHCE-GPE). This tailored special solvation structure within a polymer matrix promotes the formation of an electrochemically robust electrode-electrolyte interphase. Furthermore, employing LHCE-GPE, Li||Li(1.2)Ni(0.13)Co(0.13)Mn(0.54)O(2) cells operating at 4.8 V demonstrate a high specific capacity of 248 mAh g(-1), and 4.5 V Li||LiNi(0.8)Co(0.1)Mn(0.1)O(2) cells achieve a remarkable cycling stability over 1000 cycles. Significantly, our LHCE-GPE allows for the operation of practical solid-state 18650 cylindrical LMBs at 4.7 V and industrial Li-ion batteries at 4.6 V, achieving high energy densities of 250 and 283 Wh kg(-1), respectively (excluding packaging), while also demonstrating robust safety during rigorous nail-penetration tests. Our LHCE-GPE design presents a practical and powerful strategy for realizing solid-state LMBs with high energy density and high safety.