The electrolytes with high lithium-ion transference number (tLi+) can reduce the formation of concentration polarization during charge/discharge process and improve the electrochemical performance of lithium-ion batteries (LIBs). Herein, we report triblock copolymer electrolytes (PBOEE) containing borate. The sp2 hybridized boron atoms acting as Lewis acids can anchor the anions of lithium salts, enabling PBOEE to achieve high tLi+ of up to 0.53. Also, the borate groups can promote the formation of stable organic-rich solid electrolyte interphase (SEI) film, which enables the Li symmetric cell to cycle stably at 0.1 mA cm-2/0.1 mAh cm-2 for more than 3100 h with a low overpotential of 0.08 V under 50 °C. The optimized PBOEE_24 has an ionic conductivity of 1.41 × 10-4 S cm-1 and electrochemical stability window of 4.8 V vs. Li+/Li at 50 °C. Combining these advantages, the LiFePO4/PBOEE_24/Li cell exhibits an initial discharge specific capacity of 157.3 mA h g-1 at 0.5C with a capacity retention of 85 % after 600 cycles under 50 °C. At a higher current density of 1C, the discharge capacity maintains at 128.0 mA h g-1 after 400 cycles with a capacity retention of 84.88 %. These results suggest that block copolymer containing sp2 hybridized boron atoms is a promising all-solid-state polymer electrolyte.
Keywords: All-solid-state Li metal battery; Borate groups; Lithium-ion transport; Solid electrolyte interface; Triblock copolymer.
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