Chlorine-rich lithium argyrodites enables superior performances for solid-state Li-Se batteries at wide temperature range

All-solid-state Li-Se battery shows great potential as a candidate for next-generation energy storage devices due to its high energy density and safety.However,the low ionic conductivity of the solid electrolytes and large volume changes of Se active materials are two of the major issues that limit its applications.Herein,a simple solid-state reaction method is applied to synthesize chlorine-rich argyrodite Li_(5.5)PS_(4.5)CI_(1.5)electrolyte with high conductivity of 6.25 mS·cm^(-1)at room temperature.Carbon nanotube(CNT)is introduced as the host for Se to obtain Se/CNT composite with both enhanced electronic conductivity and lower volume expansion during the electrochemical reaction process.All-solid-state Li-Se battery using Li_(5.5)PS_(4.5)CI_(1.5)as solid electrolyte combined with Se/CNT cathode and Li-In anode shows a discharge capacity of 866 mAh·g-1for the 2nd cycle under0.433 mA·cm-2at room temperature.Moreover,the assembled battery delivers a high discharge capacity of1026 mAh·g^(-1)for the 2nd cycle when cycled at the same current density at 60℃and maintains a discharge capacity of 380 mAh·g^(-1)after 150 cycles.Owing to the high Li-ion conductivity of Li_(5.5)PS_(4.5)CI_(1.5)electrolyte,the assembled battery displays a high discharge capacity of 344 mAh·g^(-1)under 0.113 mA·cm^(-2)at-20℃C and remains 66.1%after200 cycles.In addition,this all-solid-state Li-Se battery shows ultralong cycling performances up to 1000 cycles under 0.433 mA·cm^(-2)at-20℃.This work offers the design clue to fabricate the all-solid-state Li-Se battery workable at different operating temperatures with an ultralong cycling life.

Tuning Solid Interfaces via Varying Electrolyte Distributions Enables High-Performance Solid-State Batteries

Solid/solid interface is the major challenge for high-performance solid-state batteries.Solid electrolytes(SEs)play a crucial role in the fabrication of effective interfaces in solid-state batteries.Herein,the electrolyte distribution with varied particle sizes is tuned to construct solid-state batteries with excellent performance at different operating temperatures.Solid-state batteries with the configuration S/L(small-sized SE in composite cathode and large-sized SE in electrolyte layer)show the best performance at room temperature(168 mA h g^(−1) at 0.2 C,retention of 99%,100 cycles)and−20°C(89 mA h g^(−1) at 0.05 C),while the configuration S/S displays better performance at elevated temperature.The superior performance of S/L battery is associated with faster lithium-ion dynamics due to the better solid/solid interface between active materials and electrolytes.Moreover,the inferior performance at 60℃is caused by the formation of voids and cracks in the electrolyte layer during cycling.In contrast,the S/S battery delivers superior performance at elevated operating temperature because of the integrated structure.This work confirms that tailoring electrolyte size has significant effect on fabricating all-climate solid-state batteries.