A persistent-range hydrogen-bonded gel polymer electrolyte enabling wide-temperature and recyclable lithium metal batteries

Although energy density and cycling stability remain central to lithium metal battery (LMB) research, particularly in solid-state systems, two critical yet underappreciated challenges are wide-temperature operability and recyclability. These key parameters are fundamentally governed by electrolyte design. Here, we introduce a persistent-range hydrogen-bonded (PHB) gel polymer electrolyte (GPE) for LMBs. Constructed via continuous hydrogen-bonding interactions between perfluorinated branches and ─NH─ groups on fluorinated polyurethane backbones, this dynamic network architecture synergizes seemingly incompatible properties: chemically cross-linked–level mechanical robustness and chemical stability, alongside physically cross-linked–level dynamicity and ionic conductivity (8.6 mS cm −1 in regular carbonate electrolytes). The resulting PHB-GPE endows Li-metal pouch cells with stable cycling across a −60° to 100°C temperature range. Moreover, PHB-GPE exhibits recyclability potential, enabling the reuse of the Li salt and polymer at the end of battery life. These findings provide transformative insights into designing multifunctional GPE structures for next-generation LMBs, addressing both performance and sustainability imperatives.