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The liquid‐phase synthesis (LS) of sulfide solid electrolytes (SEs) has promising potential for mass production of practical all‐solid‐state Li batteries (ASLBs). However, their accessible SE compositions are mostly metal‐free. Moreover, liquid‐phase‐synthesized‐SEs (LS‐SEs) suffer from high electronic conductivity due to carbon impurities, resulting in below‐par electrochemical performance of ASLBs. Here, the LS of highly deformable and air‐stable Li3+xP1‐xSnxS4 (0.19 mS cm−1) using 1,2‐ethylene diamine‐1,2‐ethanedithiol with tetrahydrofuran is reported. A low heat‐treatment temperature (260 °C) prevents the carbonization of organic residues. Importantly, a remarkable enhancement in the deformability of LS‐SEs compared to that of conventional solid‐state‐synthesized SEs (SS‐SEs) is identified for the first time. LiNi0.7Co0.15Mn0.15O2 electrodes employing LS‐SEs in ASLBs significantly outperform those using SS‐SEs, notably when assembled under a low fabricating pressure (148 vs 370 MPa, e.g., capacity loss: 2 vs 41 mA h g−1) or tested under a low operating pressure (12 or 3 MPa), which is attributed to reduced electrochemo‐mechanical effects. Finally, when employing SEs that are exposed to air (dew point of −20 °C), LiNi0.7Co0.15Mn0.15O2 electrodes employing SEs with Sn‐substituted composition or prepared by LS exhibit significantly better capacity retention than conventional SEs with Sn‐free composition or prepared by SS (e.g., 92.2% for LS‐Li3.2P0.8Sn0.2S4 vs 32.5% for SS‐Li3PS4). [ABSTRACT FROM AUTHOR]

The excellent stability of sulfide solid electrolytes with solvate ionic liquids Li(triethylene glycol dimethyl ether)bis(trifluoromethanesulfonyl)imide (Li(G3)TFSI), and their application for high‐performance, all‐solid‐state lithium‐ion batteries are successfully demonstrated. The addition of a small amount of Li(G3)TFSI gives an alternative ionic pathway through normally poor solid–solid contacts, leading to a dramatic increase in LiFePO4 composite electrode capacity. [ABSTRACT FROM AUTHOR]

[Display omitted] • Electrochemo-mechanical effects for all-solid-state batteries are categorized. • The mechanical properties of solid electrolytes are considered. • Stress sources, resulting cell failures, and stress cross-talks are discussed. All-solid-state batteries (ASSBs) using inorganic solid electrolytes (SEs) are in the spotlight for next-generation energy storage devices because of their potential for outstanding safety and high energy density. Recent progress in this field has been primarily based on advances in materials, such as the discovery of SEs with high ionic conductivities and the improvement of interfacial stability in electrodes. However, the use of inelastic SEs causes severe electrochemo-mechanical failures, such as cathode active material (CAM) disintegration, CAM/SE contact loss, and stress build-up during cycling, deteriorating the Li+ and e− transport pathways. Although these concerns have been addressed previously, they have not been contextualized systematically in terms of the mechanical interactions among the components and their impacts on electrochemical performance. Here, we categorize the electrochemo-mechanical effect in ASSBs and its ramifications in terms of stress sources, active materials, composite electrodes, and cell stacks. [ABSTRACT FROM AUTHOR]