The polymerization methodologies hold critical importance in fabricating high-quality gel polymer electrolytes (GPEs) for solid-state batteries. This work introduces a plasma-activated instantaneous polymerization strategy for the synthesis of initiator-free poly(ethylene glycol) diacrylate (PEGDA)-based GPEs within seconds. The N radicals produced by N2 plasma can efficiently initiate the polymerization of PEGDA monomers without requiring chemical initiators. Notably, the plasma-derived GPEs (N-GPEs) exhibit superior ionic conductivity (0.69 × 10-3 S cm-1) compared to thermally polymerized counterparts (0.42 × 10-3 S cm-1), due to the formation of optimized ion-conduction pathways. Remarkably, this initiator-free synthetic protocol demonstrates dual interfacial advantages, not only on suppression of initiator-induced side reactions at lithium metal anodes but also formation of a Li3N-enriched solid electrolyte interphase (SEI) through reactive nitrogen species, collectively enhancing the interfacial stability and ion transport kinetics. Electrochemical evaluations demonstrate that symmetric Li||Li cells with N-GPEs show stable cycling over 1600 h with minimal polarization (21 mV at 0.1 mA cm-2). When integrated into Li||LiFePO4 full cells, the system achieves 96.3% capacity retention after 200 cycles at 0.5 C, which is much better than the counterpart. This plasma-enabled polymerization technology establishes a paradigm shift in fabrication of polymer electrolyte, offering a rapid and energy-efficient route to high-performance GPEs for energy storage.
Liu et al. (Thu,) studied this question.
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