Gel polymer electrolytes (GPEs) offer a promising platform for high‐energy and safe lithium metal batteries (LMBs) by combining the ionic conductivity of liquids with the mechanical robustness of solids. However, gas evolution during in‐situ thermal polymerization often induces interfacial voids, weakening adhesion and degrading cycling stability. Here, we introduce low‐frequency mechanical vibration (5 Hz) as a facile strategy to suppress void formation and reinforce interfacial integrity. Vibration redistributes the liquid precursor and disperses nitrogen gas generated from the azo initiator, yielding a conformal, void‐free interface without altering the polymer's chemistry. This interfacial reinforcement increases adhesion energy by 54% (8.5 → 13.1 J m −2 ) and reduces charge–transfer resistance (39.9 → 23.1 Ω), enabling stable Li plating/stripping for over 300 h at 2 mA cm −2 . In Li‖LFP full cells, vibration‐treated GPEs enhance ionic transport and rate performance, delivering 118.7 mAh g −1 after 100 cycles at 1 C compared to 86.5 mAh g −1 for untreated cells. Numerical simulations further reveal that vibration promotes uniform ion flux and homogeneous Li deposition on the anode, while improved GPE coverage on the cathode ensures effective active‐material utilization. This vibration‐assisted polymerization provides an efficient interfacial engineering route toward durable, high‐performance GPE‐based LMBs.
Ryu et al. (Tue,) studied this question.