Abstract
Conventional polymer electrolytes suffer from low ionic conductivity, poor interface compatibility, low mechanical strength and certain flammability. Herein, a rigid-flexible synergistic ultrastrong nonflammable polymer electrolyte (LiNO3-PPT@PI) regulated by LiNO3 is developed, which consists of rigid polyimide (PI) fiber skeleton and flexible poly pentaerythritol tetraacrylate (PPT) plasticized with LiNO3/triethyl phosphate (TEP)/fluoroethylene carbonate (FEC). PI fiber skeleton enhances tensile strength of LiNO3-PPT@PI to 21.8 MPa. TEP effectively enhances ionic conductivity to 7.57 × 10−4 S cm−1 at 30 °C and improves flame retardancy. LiNO3 is creatively utilized as the only lithium salt for LiNO3-PPT@PI to construct Li3N-rich solid electrolyte interphases (SEIs) and promote FEC to form LiF-rich SEIs/cathode-electrolyte interphases (CEIs) to improve interface stability, thereby enabling high-efficiency, long-term and dendrite-free cycling of LiFePO4 (LFP)||Li cells and LiNi0.8Mn0.1Co0.1O2 (NCM811)||Li cells, which is superior to the LiPF6-based polymer electrolytes. LFP||Li cells with LiNO3-PPT@PI exhibit excellent cycle performance over 650 cycles with 81.8 % capacity retention. This work presents a promising design strategy of safe and efficient polymer electrolytes for Li metal batteries.
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