A smart lithiophilic polymer filler in gel polymer electrolyte enables stable and dendrite-free Li metal anode

The Li-metal anode plays a critical role in meeting the ever-growing demands for high-energy-density batteries. The rational design of an electrolyte to suppress dendrite formation is of great significance for the practical use of a Li-metal anode in rechargeable Li-metal batteries. In this work, by taking advantage of the lithiophilic polyacenequinone polymer filler, a novel polymer-filler-reinforced gel polymer electrolyte with the merits of high mechanical flexibility, high ionic conductivity, and superior dendrite-Li suppressing ability has been developed. When this gel polymer electrolyte is used in Li symmetrical cells, small and stable Li-plating/stripping overpotentials (~25 mV) can be maintained over 700 hours. When equipped with a high-voltage cathode of LiNi_0.6Co_0.2Mn_0.2O₂(NCM622) for Li-metal batteries, a high coulombic efficiency of about 99% can be retained after 100 repeated cycles. Such superiority is mainly ascribed to the smart lithiophilic carbonyl groups on the polyacenequinone polymer filler, which can guide uniform Li-ion flux at the Li electrode/electrolyte interface to fundamentally suppress Li dendrite growth during cycling. This work paves a way for designing dendrite-suppressed gel polymer electrolytes for Li-metal batteries and related energy conversion and storage devices.