Self-healing and shape-memory solid polymer electrolytes with high mechanical strength facilitated by a poly(vinyl alcohol) matrix

Self-healing and shape-memory solid polymer electrolytes (SSSPEs) based on poly(vinyl alcohol) (PVA) with ureidopyrimidinone (UPy) and poly(ethylene glycol) (PEG) units (PVA-UPy-PEG) were successfully fabricated by the reactions of different chain length epoxide functionalized-PEG and 2(6-isocyanatohexylaminocarbonylamino)-6-methyl-4[1 H ]-pyrimidinone (UPy-NCO) with the hydroxyl of PVA. The SSSPE with the longest PEG side chain (PVA-UPy-PEG750) exhibited good thermal stability until 254 C, a low glass transition temperature (44.8 C), excellent self-healing and shape-memory performance, and high tensile stress. The PVA-UPy-PEG750 also showed a high ionic conductivity of 1.51 10 4 S cm 1 with an EO/Li + ratio of 11:1 at 60 C, wide electrochemical window (5.0 V vs. Li/Li + ), and improved lithium-ion transference number ( t Li + = 0.34). Moreover, the lithium plating/stripping behavior of SSSPEs indicated the improved interfacial stability between the polymer electrolyte and the lithium metal electrode. The Li/PVA-UPy-PEG750/LiFePO 4 cell exhibited a higher initial discharge capacity of 145 mA h g 1 and maintained a discharge capacity of 117 mA h g 1 after 150 cycles and a coulombic efficiency of 99% with 0.1C at 60 C. The SSSPE could be a promising candidate as the all-solid-state polymer electrolyte for lithium-ion batteries. This article reports PVA-based electrolytes with supramolecular networks formed via quadruple hydrogen bonding for lithium-ion batteries.