Abstract

High-energy rechargeable sodium metal batteries, featuring quasi-solid polymer electrolytes (QSSPEs), hold the promise of improved safety. However, the low ionic conductivity and limited cyclability of QSSPEs at room temperature have paralyzed the efforts to develop energy-dense metal anode batteries. Herein, we report a QSSPE comprising a blend of polyvinyl pyrrolidone (PVP) and polyethylene glycol (PEG). Notably, the porosity and the electrolyte uptake capacity of the QSSPE are highly responsive to the concentration of PEG. The optimized PVP-based QSSPE (PVP-PEG 70 30) shows a high ionic conductivity of 1.06 mS cm−1 at room temperature, along with a high transference number of approximately 0.81. A sodium symmetric cell using PVP-PEG 70 30 demonstrates reversible stripping/plating of sodium for over 700 h at a current density of 1 mA cm−2. Furthermore, PVP-PEG 70 30 alters the localized chemistry of the solid electrolyte interphases (SEIs), facilitating the formation of fluorine-rich SEIs. When coupled with a Prussian blue cathode and sodium metal anode, a full cell employing PVP-PEG 70 30 exhibits an initial discharge capacity of 168 mAh g−1, with an average discharge capacity of 125 mAh g−1 for over 600 cycles at 0.5C. Remarkably, this cell can be cycled stably and reversibly at a high rate of 6.5C. These results suggest that PVP-based QSSPE holds great promise as an electrolyte candidate for high-performance sodium metal batteries.

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