In-situ generated solid-state electrolytes with intimate interface affinity enable conductivity and high performances for lithium-ion batteries

Abstract

The issues of interfacial compatibility derived from electrolyte/electrodes and unsatisfied ionic conductivity still hinder the practical application of lithium-ion batteries. In the present study, the crosslinked solid polymer electrolytes (SPEs) based on dual epoxy group were prepared through in-situ thermal polymerization method. FSO2NH2 was employed as additive for high reactivity to adapt the kinetic reaction and improve the conductivities of electrolytes. The as-prepared SPEs exhibit a high degree of amorphous structure, lower transmission glass temperature, considerable ionic conductivity (>1.0 mS cm−1) at 25 °C, wider electrochemical stability window, and excellent Li cation transference number. Moreover, the battery performance of the as-prepared PBDE−1 electrolyte-based half-cell means that it delivers a high initial specific capacity (ca. 161.2 mAh g−1), and achieves remarkable Coulombic efficiency of 99.8% after 200 cycles at 0.1 C. X-ray photoelectron spectra further revealed the formation of a solid electrolyte interphase (SEI) layer, which can alleviate Li dendrite growth and facilitate the lifespan stability of Li/graphite anode during cycling. These findings may provide a reference for the development of solid-state lithium batteries.