SiSe2 for Superior Sulfide Solid Electrolytes and Li-Ion Batteries.

Abstract

Among the various existing layered compounds, silicon diselenide (SiSe2) possesses diverse chemical and physical properties, owing to its large interlayer spacing and interesting atomic arrangements. Despite the unique properties of layered SiSe2, it has not yet been used in energy applications. Herein, we introduce the synthesis of layered SiSe2 through a facile solid-state synthetic route and demonstrate its versatility as a sulfide solid electrolyte (SE) additive for all-solid-state batteries (ASSBs) and as an anode material for Li-ion batteries (LIBs). Li-argyrodites with various compositions substituted with SiSe2 are synthesized and evaluated as sulfide SEs for ASSBs. SiSe2-substituted Li-argyrodites exhibit high ionic conductivities, low activation energies, and high air stabilities. In addition, when using a sulfide SE, the ASSB full cell exhibits a high discharge/charge capacity of 202/169 mAh g-1 with a high initial Coulombic efficiency (ICE) of 83.7% and stable capacity retention at 1C after 100 cycles. Furthermore, the Li-storage properties of SiSe2 as an anode material for LIBs are evaluated, and its Li-pathway mechanism is explored by using various cutting-edge ex situ analytical tools. Moreover, the SiSe2 nanocomposite anode exhibits a high Li- insertion/extraction capacity of 950/775 mAh g-1, a high ICE of 81.6%, a fast rate capability, and stable capacity retention after 300 cycles. Accordingly, layered SiSe2 and its versatile applications as a sulfide SE additive for ASSBs and an anode material for LIBs are promising candidates in energy storage applications as well as myriad other applications.