Cold-pressing PEO/LAGP composite electrolyte for integrated all-solid-state lithium metal battery

Polyethylene-oxide (PEO)-based electrolyte is one of the most promising solid electrolytes due to its outstanding safety and excellent flexibility. However, the most common method to fabricate PEO-based electrolyte is casting, which requires intensive use of toxic organic solvent. Besides, the agglomeration of filler in the composite electrolyte fabricated by casting limits further enhancement of ionic conductivity. In this work, we provide a facile solvent-free cold-pressing method to prepare well-dispersed LAGP @ PEO composite solid-state electrolyte. The ionic conductivity of LAGP @ PEO composite electrolyte can reach about 4.4 × 10−5 S cm−1 at room temperature which is nearly one order of magnitude higher than that of the casting one (3.3 × 10−6 S cm−1). The integrated all-solid-state batteries display excellent cycling stability and good rate performance at 50 °C. Our work provides a facile solvent-free cold-pressing method to fabricate polymer-based composite electrolyte with well-dispersed filler for all-solid-state batteries. [Display omitted] •Well-dispersion of solid state electrolyte in PEO via facile method•Improved adhesion ascribed to the synergistic effect of PEO and PVDF.•Environmental friendly fabrication based on the solvent-free process