The incorporation of solid-state electrolytes (SSEs), which exhibit electronic insulation properties but also high ionic conductivities, has been considered an effective strategy for tackling the high-temperature instabilities of non-aqueous alkali metal-based batteries 3. However, the high flammability and easy leakage of organic liquid electrolytes result in safety challenges for SIBs. Owing to the availability of Na and its physicochemical properties, sodium-ion batteries (SIBs) are regarded as a primary alternative for lithium-ion batteries (LIBs), especially in large-scale and distributed energy storage systems 1, 2. Testing the quasi-solid-state electrolyte in Na||Na 3V 2(PO 4) 3 coin cell configuration demonstrates fast reaction dynamics, low polarization voltages, and a stable cycling performance over 1000 cycles at 60 mA g –1 and 25 ± 1 ☌ with a 0.0048% capacity decay per cycle and a final discharge capacity of 83.5 mAh g −1. The quasi-solid-state electrolyte enables selective Na + transport along specific areas that are electronegative with sub-nanometre dimensions, resulting in a Na + conductivity of 1.30×10 –4 S cm –1 and oxidative stability of up to 5.32 V (versus Na +/Na) at 25 ± 1 ☌. Herein, inspired by the Na +/K + conduction in biological membranes, we report a (–COO –)-modified covalent organic framework (COF) as a Na-ion quasi-solid-state electrolyte with sub-nanometre-sized Na + transport zones (6.7–11.6 Å) created by adjacent –COO – groups and COF inwalls. However, moderate ionic conductivity and narrow electrochemical windows hinder their further application. Solid polymer electrolytes are considered among the most promising candidates for developing practical solid-state sodium batteries.
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