A hybrid lithium sulfonated polyoxadiazole derived single-ion conducting gel polymer electrolyte enabled effective suppression of dendritic lithium growth

Lithium metal is deemed as an ideal anode material in lithium-ion batteries because of its ultrahigh theoretical specific capacity and the lowest redox potential. However, the rapid capacity attenuation and inferior security resulting from the dendritic lithium growth severely limit its commercialization. Herein a novel hybrid gel polymer electrolyte (GPE) based on electrospun lithium sulfonated polyoxadiazole (Li-SPOD) nanofibrous membrane swelled by lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) ether liquid electrolyte is proposed to address the issue of lithium dendrites. The Li-SPOD membrane synthesized by a simple one-pot method exhibits excellent mechanical strength and thermal resistance due to its high molecular weight and rigid backbone. The electron-withdrawing oxadiazole ring and oxadiazole ring-Li⁺ complex, and N, O heteroatoms with lone pairs of electrons in Li-SPOD macromolecular chains facilitate the dissociation of -SO₃Li group and Li⁺ transference. The hybrid Li-SPOD GPE exhibits both a high lithium-ion transference number (0.64) and high ionic conductivity (2.03 mS/cm) as well as superior interfacial compacity with lithium anodes. The LiFePO₄-Li cell using this novel GPE can operate steadily at 2 C for 300 cycles, remaining a high discharge capacity of 125 mAh/g and dendrite-free anode. Remarkable performance improvements for the Li-Li and Cu-Li cells are also presented.