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LIBs) are desirable to significantly increase to fulfill the growing demand for long distance per each charge. For this reason, next generation batteries such as Li-S, Li-O 2 , and Li-metal with exceptional energies have been attracted much attention as potential candidates due to their outstanding performances. [1][2][3][4][5] However, unfortunately, as a substantial amount of electrochemical energy should be stored in a confined volume, these systems are thermodynamically unstable, which could be a risk for safety incidents.In an attempt to overcome these drawbacks, the all-solid-state batteries (ASSBs) with all-solidified components are now considered as a promising next-generation technology beyond state-of-the-art LIBs. [6] The fascinating features of the ASSBs lie in the opportunity of enhancing energy density and surmounting the intrinsic shortcomings of conventional liquid-based batteries, such as electrolyte leakage, flammability, narrow voltage window, and low lithium ion transport number. In other words, the ASSBs are promising systems due to nonvolatile, nonexplosive, and stability up to ≈6.0 V versus Li/Li + . [6][7][8][9][10] In particular, if lithium metal can be employed as an anode material and interfacial stability can be improved, [11,12] it can be possible to achieve high energy and power density. These extraordinary properties of the ASSBs have extensively stimulated scientific and industry communities to the ASSB's research.In order to achieve superior electrochemical performances of the ASSBs, not only improving interfacial stability during the cycling, but balancing both ionic and electronic conductivities of composites is of crucial importance. For instance, while the electronic pathways appear to be more important for the high energy density ASSBs operating at relatively low current density, the sufficient ion transport is a more critical factor at high rate operations for the high power density ASSBs, [13,14] although the cell performances are relatively related to diverse factors such as the operating pressure/temperature, particle size, and composition in the electrode. In terms of enhancement of the ionic conductivity, extensive efforts for developing solid electrolyte (SE) with high ionic conductivity have been conducted for past few decades. Among diverse candidates, much attention has been focused on the sulfide-based SE including Li 10 GeP 2 S 12 (LGPS), [7,15] β-Li 3 PS 4 , [16] Li 7 P 3 S 11 , [17] Li 2 S-P 2 S 5 , [18] and argyrodite All-solid-state batteries (ASSBs) have lately received enormous attention for electric vehicle applications because of their exceptional stability by engaging all-solidified cell components. However, there are many formidable hurdles such as low ionic conductivity, interface instability, and difficulty in the manufacturing process, for its practical use. Recently, carbon, one of the representative conducting agents, turns out to largely participate in side reactions with the solid electrolyte, which finally leads to the formation of insulating sid...

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All-solid-state batteries (ASSBs) comprising solidified cathodes, electrolytes, and Li-metal anodes have attracted notable attention as promising future batteries for electric vehicles owing to their exceptional stability and expectation of achieving high energy density. However, its permanent operation has been hindered by Li dendrite growth, chemo-mechanical degradation, and interfacial instability, leading to Li exhaustion, increased resistance, and internal short-circuiting. Herein, for the first time, the authors report the effects of a lithium nitride (Li 3 N) sacrificial cathode on the cycling performance of ASSBs combined with a Li-free In layer. Through in situ evolved gas and internal pressure change analyses of the cells, it is found that, as with the liquid electrolyte cell, the decomposed Li 3 N compensates for active Li consumed by side reactions in the cell. Moreover, it is demonstrated that the improved interparticle contact by volume expansion of In through additionally supplied Li as well as the interfacial stability at the anode side by the dendrite-free In layer, are strongly responsible for the improved cyclability of the ASSBs. The findings reveal the effectiveness of the Li compensation approach for the stable cycling of ASSBs based on the secured interfacial stability at the anode side.

With the timely advent of the electric vehicle era, where battery stability has emerged as a major issue, all-solid-state batteries (ASSBs) have attracted significant attention as the game changer owing to their high stability. However, despite the introduction of a densely packed solid electrolyte (SE) layer, when Li is used to increase the energy density of the cell, the short-circuit problem caused by Li protrusion is unavoidable. Furthermore, most strategies to control nonuniform Li growth are so complicated that they hinder the practical application of ASSBs. To overcome these limitations, this study proposes an Ag-Li alloy anode via mass-producible roll pressing method. Unlike previous studies reporting solid-solution-based metal alloys containing a small amount of lithiophilic Ag, the in situ formed and Ag-enriched Ag-Li intermetallic layer mitigates uneven Li deposition and maintains a stable SE/Ag-Li interface, facilitating reversible Li operation. Contrary to Li cells showing frequent initial short-circuit, the cell incorporating the Ag-Li anode exhibits a better capacity retention of 94.3% for 140 cycles, as well as stable cycling even under 12 C. Through a facile approach enabling the fabrication of a large-area anode with controllable Li growth, this study provides practical insight for developing ASSBs with stable cyclabilities.