A series of new self-standing gel polymer electrolytes (SGPEs) were fabricated by ultraviolet (UV) curing and investigated for application in flexible lithium-ion batteries. Compared with traditional gel polymer electrolytes (combine with solvents or plasticizers), these new SGPEs were prepared simply by curing different weight ratios of lithium bis(fluorosulfonyl)imide (LiFSI) with a methacrylic linear monomer, poly (ethylene glycol) dimethacrylate (PEGDMA). Noticeably, there were no solvents or plasticizers combined with the final SGPEs. Owing to this, the SGPEs showed high flexibility and strong mechanical stability. Some paramount physicochemical and electrochemical characters were observed. The SGPEs demonstrated good thermal stability below 150 °C and an extremely low glass transition temperature (T_g) (around −75 °C). Moreover, plastic crystal behaviors were also identified in this study. Ultimately, the SGPEs demonstrated excellent ionic conductivity at room temperature, which proves that these new SGPEs could be widely applied as a prospective electrolyte in flexible lithium-ion batteries.

The polymer electrolytes are considered to be an alternative to liquid electrolytes for lithium-ion batteries because of their high thermal stability, flexibility, and wide applications. However, the polymer electrolytes have low ionic conductivity at room temperature due to the interfacial contact issue and the growing of lithium dendrites between the electrolytes/electrodes. In this study, we prepared gel polymer electrolytes (GPEs) through an in situ thermal-induced cationic ring-opening strategy, using LiFSI as an initiator. As-synthesized GPEs were characterized with a series of technologies. The as-synthesized PNDGE 1.5 presented good thermal stability (up to 150 °C), low glass transition temperature (T_g < −40 °C), high ionic conductivity (>10⁻⁴ S/cm), and good interfacial contact with the cell components and comparable anodic oxidation voltage (4.0 V). In addition, PNGDE 1.5 exhibited a discharge capacity of 131 mAh/g after 50 cycles at 0.2 C and had a 92% level of coulombic efficiency. Herein, these results can contribute to developing of new polymer electrolytes and offer the possibility of good compatibility through the in situ technique for Li-ion batteries.

Rechargeable lithium-ion batteries have drawn extensive attention owing to increasing demands in applications from portable electronic devices to energy storage systems. In situ polymerization is considered one of the most promising approaches for enabling interfacial issues and improving compatibility between electrolytes and electrodes in batteries. Herein, we observed in situ thermally induced electrolytes based on an oxetane group with LiFSI as an initiator, and investigated structural characteristics, physicochemical properties, contacting interface, and electrochemical performances of as-prepared SPEs with a variety of technologies, such as FTIR, ¹H-NMR, FE-SEM, EIS, LSV, and chronoamperometry. The as-prepared SPEs exhibited good thermal stability (stable up to 210 °C), lower activation energy, and high ionic conductivity (>0.1 mS/cm) at 30 °C. Specifically, SPE-2.5 displayed a comparable ionic conductivity (1.3 mS/cm at 80 °C), better interfacial compatibility, and a high Li-ion transference number. The SPE-2.5 electrolyte had comparable coulombic efficiency with a half-cell configuration at 0.1 C for 50 cycles. Obtained results could provide the possibility of high ionic conductivity and good compatibility through in situ polymerization for the development of Li-ion batteries.