Lithium argyrodites electrolyte with high ionic conductivity and relatively lower cost show great potential as candidates for solid-state batteries. Further improvement of their conductivities can accelerate their applications. One of the means to significantly promote the conductivity of Li-ion is dual doping. Herein, Ag/Br dual-doping strategy is applied on Li 6 PS 5 Br (2.76 mS cm −1 ) to boast its conductivity to 6.15 mS cm −1 for Li 5.55 Ag 0.05 PS 4.6 Br 1.4 . The structural variations and chemical/electrochemical stability of the obtained electrolyte are carefully investigated. Li 3 InCl 6 electrolyte is introduced in the new battery configuration to mitigate the interfacial instability with LiNi 0.6 Mn 0.2 Co 0.2 O 2 active material enabling good electrochemical performances . The assembled battery delivers a discharge capacity of 160.8 mAh g −1 for the 1st cycle and maintains 85.9% of the initial value after 50 cycles at 0.5C. This modification strategy was proved effective for increasing the conductivity of sulfide electrolytes in this work.
The sulfide electrolyte-based all-solid-state batteries with high-nickel layered oxide cathodes face significant challenges due to the narrow electrochemical window of sulfides and severe side reactions caused by direct contact with high-voltage oxide cathode materials such as LiNi 0.9 Mn 0.05 Co 0.05 O 2 (NCM90). Here, we successfully synthesized Li 3 InCl 6 (LIC) halide electrolytes through ball-milling followed by annealing method, achieving the ionic conductivity of 2.0 mS cm −1 at room-temperature. The interface between this electrolyte and NCM90 cathode material without any interface modification is stable. By introducing the LIC electrolyte layer, the NCM90/LIC+Cl1.5/Li-In battery exhibits significantly improved electrochemical performance at different temperatures, particularly in terms of initial discharge capacity. Notably, the battery demonstrates outstanding discharge capacity and cycling stability at low temperatures. Experimental investigations reveal that the introduction of the LIC electrolyte with high oxidation potential facilitates the H2-H3 phase transition in NCM90 during high-voltage operation, which is critical for enhancing the discharge capacity. This work provides fundamental insights into interfacial engineering strategies for high-voltage sulfide-based all-solid-state battery systems.
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