Soluble and perfluorinated polyelectrolyte for safe and high-performance Li-O${}_2$ batteries

The severe performance degradation of high-capacity Li-O${}_2$ batteries induced by Li dendrite growth and concentration polarization from the low Li${}^{+}$ transfer number of conventional electrolytes hinder their practical applications. Herein, lithiated Nafion (LN) with the sulfonic group immobilized on the perfluorinated backbone has been designed as a soluble lithium salt for preparing a less flammable polyelectrolyte solution, which not only simultaneously achieves a high Li${}^{+}$ transfer number (0.84) and conductivity (2.5 mS cm${}^{-1}$), but also the perfluorinated anion of LN produces a LiF-rich SEI for protecting the Li anode from dendrite growth. Thus, the Li-O${}_2$ battery with a LN-based electrolyte achieves an all-round performance improvement, like low charge overpotential (0.18 V), large discharge capacity (9508 mAh g${}^{-1}$), and excellent cycling performance (225 cycles). Besides, the fabricated pouch-type Li-air cells exhibit promising applications to power electronic equipment with satisfactory safety. (© 2022 Wiley‐VCH GmbH)