Integrated manufacturing of REciclable multi-material COmposites for the TRANSport sector

Oxygen?vacancy lithium zirconate (O?LZO) reduces the bonding between lithium ion (Li+) and anions in lithium salts, promoting dissociation and increasing the concentration of free Li+. Kinetic simulations confirm the excellent intrinsic Li+ diffusion capability of O?LZO. As an active filler, O?LZO broadens Li+ transport pathways and enhances the dissociation and distribution of lithium salts, improving overall electrolyte performance.The low concentration and inhomogenous distribution of free lithium ion (Li+) in composite polymer electrolytes (CPEs) greatly restrict the Li+ transport, cycle stability and rate performance of all solid?state batteries. In this work, lithium zirconate with superficial oxygen (O)?vacancies (O?LZO) is reported as a new Li+ conductors for polyethylene oxide (PEO)?based CPEs (PEO@O?LZO). The O?LZO demonstrates exceptional Li+ transport capability, and its superficial O?vacancies efficiently adsorb anions to facilitate the dissociation of lithium salts, leading a high concentration of free Li+ in CPEs. Furthermore, the electropositive equilibrium charge layer of O?vacancies avoids the aggregation of Li+ near the filler and achieves a stable interface to promote the efficient and continuous Li+ transport. These effects contribute to a high Li+ conductivity of 1.63 × 10?4 S cm?1 and a Li+ migration number of 0.35 for PEO@O?LZO at 40 °C. The assembled battery (LiFePO4/PEO@O?LZO/Li) exhibits a capacity of 120 mAh g?1 at 3 C and stable cycling performance with an 80.5% capacity retention after 800 cycles at 1 C and 40 °C, maintaining excellent coulombic efficiency. This work provides a design principle of fillers to regulate Li+ concentration and distribution in CPEs for efficient solid?state lithium metal batteries.

» Publication Date: 22/05/2025

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