Unlocking high lithium-ion transport in solid polymer electrolytes with dynamic hydrogen-bonded zinc-adeninate framework

Summary Fast and selective lithium-ion transport is crucial for advancing solid-state electrolytes in lithium metal batteries. While porous materials with tunable Li+ transport pathways show promise, challenges remain in optimizing transport kinetics, stability, and interfacial compatibility. Herein, we present a solid-state polymer electrolyte (SPE) incorporating a hydrogen-bonded zinc-adeninate framework (ZAF) with abundant carbonyl and hydrogen-bonding functionalities, providing additional hopping sites for Li+ transport. The ZAF-poly(ethylene oxide) (PEO) electrolyte achieves high ionic conductivity (1.37 mS cm−1 at 60°C), a lithium-ion transfer number of 0.56, and a wide electrochemical window (5.04 V). It delivers exceptional cycling stability, with Li|ZAF-PEO|Li symmetric cells cycling for 1,900 h at 0.2 mA cm−2 and Li|ZAF-PEO|LFP cells stable for over 800 cycles at 1 C with 99.8% coulombic efficiency. Additionally, the pouch cell maintains excellent safety under mechanical stresses, such as bending and shearing. These results highlight the potential of ZAF-based SPEs for safer, high-performance lithium metal batteries.