Li-ion batteries (LIBs) have high energy density and long-cycle energy storage; hence, they are widely used as power sources in electric devices. However, safety remains a major issue. Conventional LIBs developed using organic, liquid electrolytes may exhibit issues such as combustion and explosion. To address these issues, all-solid-state batteries (ASSBs) are considered promising candidates for advanced LIBs, offering high electrochemical stability and excellent safety owing to the non-flammability of the intrinsic inorganic solid electrolyte used1. The deployment of solid-state electrolytes (SSEs) into all-solid-state Li batteries is a promising approach due to the non-flammability and compatibility of SSEs with Li metal; thus, they have the potential to meet the increasing demands for high energy density and enhanced safety. Among the various SSEs, Li7La3Zr2O12 (LLZO) can be doped with Al, Ga, Ta, etc., to stabilize its cubic structure. LLZO exhibits high ionic conductivities (in the range of 10−4–10−3 S·cm−1), a wide operating voltage window, and excellent elastic and shear moduli. However, all ASSBs have solid-state electrode structures consisting solely of solid materials. As a result, Li-ion diffusion primarily occurs at the interfaces between the cathode-active material and solid electrolyte. Composite cathodes within ASSBs often exhibit numerous voids and high interfacial resistance. The limited ion conduction paths have constrained the electrochemical performance of ASSBs because of the inadequate contact areas between the active materials and solid electrolytes in the composite cathode2. To improve the electrochemical performance of ASSBs, some design issues of the composite cathode electrode need to be solved. The aim of this study is to enhance the performance of ASSBs using a bimodal garnet-type solid electrolyte, Li7La3Zr2O12 (LLZO), composed of electrolytes of two different sizes. The bimodal electrolyte composite cathode exhibits a higher density and fewer voids compared to the monomodal electrolyte, as the small powder particles fill the voids between the large ones.3 Finally, ASSBs prepared using the bimodal electrolyte achieve a low interface resistance and a large contact area between the solid electrolyte and the cathode material, resulting in enhanced electrochemical performance. Further details regarding the electrochemical and structural properties will be presented in the meeting.
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