terms of safety and the ability to use highcapacity anodes, such as lithium metal, thereby attracting interest in the realization of high-energy density solid-state batteries (SSBs). [3][4][5][6][7][8] Sulfide solid electrolytes are especially promising and advanced systems for industrial application owing to their high ionic conductivity (exceeding that of liquid electrolytes), high mechanical deformability, and low gravimetric density. [9][10][11][12] However, sulfide SEs suffer from chronic interfacial issues at the cathode-SE interfaces such as chemical degradation caused by side reactions due to the low oxidation stability of the S 2− anion [13][14][15] and a common issue of the mechanical contact loss between the cathode and SE due to the volume change of the cathode during galvanostatic cycling. [16][17][18] Conventionally, oxide-based inorganic compounds with electronic-insulating and ionic-conducting character have been mainly proposed as the cathode coating layer to solely resolve cathode-SE chemical degradation. [19,20] Representatively, LiNbO 3 and Li 2 ZrO 3 and their derivatives have been widely used and studied, with mitigated chemical degradation verified, suggesting improved cycle stability. However, the chemical-degradation-induced increase in the electronic resistance or diffusion of the cation in the cathode (i.e., Co for LiCoO 2 ) to the solid electrolyte is still not fully suppressed. [21][22][23] To design a coating material with better compatibility in both the oxide-based cathode and sulfide-based solid electrolyte, material screening with density functional theory (DFT) calculation has been attempted, considering further phase stability and electrochemical stability. [10,24] A few materials have been suggested within the set criteria; however, achieving uniform coverage of the materials with target composition and structure on the cathode is unexpectedly difficult given the monotonous application process of solid-state reaction at moderate temperature (300-500 °C) after solution-based precursor mixing and drying on the cathode surface. [25][26][27] Limiting the reaction temperature to exclude side reactions with the cathode material can instead induce discrepancies in the structure and composition from the target material; thus, it is difficult to achieve the original properties predicted from the DFT calculation. In addition, although the mechanical properties of the cathode coating layer have rarely been considered in the field of SSBs thus far, the high stiffness of oxide-based inorganic compounds could result in vulnerability to chemical degradation due to crack formation Keeping both the chemical and physical state of the electrode-electrolyte interface intact is one of the greatest challenges in achieving solid-state batteries (SSBs) with longer cycle lives. Herein, the use of organic electrolyte additives in the cathode electrolyte interphase (CEI) layer to mitigate the intertwined chemical and mechanical degradation in sulfide-based SSBs is demonstrated. Lithium difluorobis(oxala...
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