Synergistic Effect and Enhanced Safety of Double Dynamic Solid Polymer Electrolytes for Lithium Metal Batteries

A solid polymer electrolyte with low mechanical strength and poor flexibility will cause mechanical degradation, short circuits, or functional failures in lithium ion batteries (LIBs). Therefore, introducing an double dynamic solid polymer electrolytes with high ionic conductivity, good mechanical strength, and excellent self-healing ability for stabilizing the solid electrolyte interface, preventing battery fire, and suppressing Li dendrite growth will further improve the reliability, security, and lifetime of the LIBs. Herein, a series of dual dynamic self-healing solid polymer electrolytes (DD-shSPEs) are developed via the Schiff base reaction between different molar ratios of polyethylene glycol derivative (tat-PEG) and terephthalaldehyde. The hydrogen bond and the highly reversible imine bonds endow DD-shSPEs with rapid self-repairing capacity to cure mechanical damage within 5 min at normal temperature. The self-healing polymer electrolytes also exhibit excellent stretchability, which can satisfy the external deformation of the battery. Meanwhile, after self-healing, the ionic conductivities of the electrolytes can hold the original values. Also, the initial discharge capacity (IDC) of the battery based on DD-shSPEs reach to 149.3 mAh g-1 under a current rate of 0.1 C, and still maintains 144.2 mAh g-1 after 100 cycles. Besides, the polymer electrolyte (PE) also exhibits good interfacial stability and have a cycle life of more