Enhancing mechanical properties of composite solid electrolyte by ultra-high molecular weight polymers

Composite solid electrolytes combining the advantages of inorganic and polymer electrolytes are considered as one of the promising candidates for solid-state lithium metal batteries. Compared with ceramic-in-polymer electrolyte, polymer-in-ceramic electrolyte displays excellent mechanical strength to inhibit lithium dendrite. However, polymer-in-ceramic electrolyte faces the challenges of lack of flexibility and severely blocked Li⁺transport. In this study, we prepared polymer-in-ceramic film utilizing ultra-high molecular weight polymers and ceramic particles to combine flexibility and mechanical strength. Meanwhile, the ionic conductivity of polymer-in-ceramic electrolytes was improved by adding excess lithium salt in polymer matrix to form polymer-in-salt structure. The obtained film shows high stiffness (10.5 MPa), acceptable ionic conductivity (0.18 mS cm^-1) and high flexibility. As a result, the corresponding lithium symmetric cell stably cycles over 800 h and the corresponding LiFePO₄cell provides a discharge capacity of 147.7 mAh g^-1at 0.1 C without obvious capacity decay after 145 cycles.