Design and Synthesis of Cubic K3−2xBaxSbSe4 Solid Electrolytes for K–O2 Batteries

Abstract

Developing K-ion conducting solid-state electrolytes (SSEs) plays a critical role in the safe implementation of potassium batteries. In this work, a chalcogenide-based potassium ion SSE is reported, K3SbSe4, which adopts a trigonal structure at room temperature. Single-crystal structural analysis reveals a trigonal-to-cubic phase transition at the low temperature of 50 °C, which is the lowest among similar compounds and thus provides easy access to the cubic phase. The substitution of barium for potassium in K3SbSe4 leads to the creation of potassium vacancies, expansion of lattice parameters, and a transformation from a trigonal phase to a cubic phase. As a result, the maximum conductivity of K3−2xBaxSbSe4 reaches around 0.1 mS cm−1 at 40 °C for K2.2Ba0.4SbSe4, which is over two orders of magnitude higher than that of undoped K3SbSe4. This novel SSE is successfully employed in a K–O2 battery operating at room temperature where a polymer-laminated K2.2Ba0.4SbSe4 pellet serves as a separator between the oxygen cathode and the potassium metal anode. Effective protection of the K metal anode against corrosion caused by O2 is demonstrated.