An entanglement association polymer electrolyte for Li-metal batteries.

Wang, Hangchao; Yang, Yali; Gao, Chuan; Chen, Tao; Song, Jin; Zuo, Yuxuan; Fang, Qiu; Yang, Tonghuan et al. · Nat Commun · 2024

basic_science · Level V

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Abstract

To improve the interface stability between Li-rich Mn-based oxide cathodes and electrolytes, it is necessary to develop new polymer electrolytes. Here, we report an entanglement association polymer electrolyte (PVFH-PVCA) based on a poly (vinylidene fluoride-co-hexafluoropropylene) (PVFH) matrix and a copolymer stabilizer (PVCA) prepared from acrylonitrile, maleic anhydride, and vinylene carbonate. The entangled structure of the PVFH-PVCA electrolyte imparts excellent mechanical properties and eliminates the stress arising from dendrite growth during cycling and forms a stable interface layer, enabling Li//Li symmetric cells to cycle steadily for more than 4500 h at 8 mA cm<sup>-2</sup>. The PVCA acts as a stabilizer to promote the formation of an electrochemically robust cathode-electrolyte interphase. It delivers a high specific capacity and excellent cycling stability with 84.7% capacity retention after 400 cycles. Li<sub>1.2</sub>Mn<sub>0.56</sub>Ni<sub>0.16</sub>Co<sub>0.08</sub>O<sub>2</sub>/PVFH-PVCA/Li full cell achieved 125 cycles at 1 C (4.8 V cut-off) with a stable discharge capacity of ~2.5 mAh cm<sup>-2</sup>.