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International audience; Li-ion batteries are the key stones of electric vehicles, but with the emergence of solid-state Li batteries for improving autonomy and fast charging, the need for mastering the solid electrolyte (SE)/electrode material interfaces is crucial. All-solid-state-batteries (ASSBs) suffer from long-term capacity fading with enhanced decomposition reactions. So far, these reactions have not been extensively studied in Li(6)PS(5)Cl-based systems because of the complexity of overlapping degradation mechanisms. Herein, those reactions are studied in depth. We investigated their effects under various operating conditions (temperature, C-rate, voltage window), types of active materials, and with or without carbon additives. From combined resistance monitoring and impedance spectroscopy measurements, we could decouple two reactions (NMC/SE and VGCF/SE) with an inflection dependent on the cutoff potential (3.6 or 3.9 V vs Li-In/In are studied) on charge and elucidate their distinct repercussions on cycling performances. The pernicious effect of carbon additives on both the first cycle and power performances is disclosed, so as its long-term effect on capacity retention. As a mean to resolve these issues, we scrutinized the benefits of a coating layer around NMC particles to prevent high potential interactions, minimize the drastic loss of capacity observed with bare NMC, and simply propose to get rid of carbon additives. Altogether, we hope these findings provide insights and novel methodologies for designing innovative performing solid-state batteries.

Lithium-ion batteries (LIBs) are widely used in portable electronic devices, electric vehicles and large scale energy storage, due to their considerable energy density, low cost and long cycle life. However, traditional liquid batteries suffer from safety problems such as leakage, thermal runaway and even explosion. Part of the issues are caused by lithium dendrites puncturing the liquid electrolyte during cycling. In order to achieve the objective of higher safety and energy density, a rigid solid-state electrolyte (SSE) is proposed instead of liquid electrolyte (LE). Thereinto, sulfide SSEs have received of the most attention due to their high ionic conductivity. Among all the sulfide SSEs, argyrodite SSEs are considered to be one of the most promising solid-state electrolytes due to their high ionic conductivity, high thermal stability and good processablity. On the other hand, lithium metal is an ideal material for anode because of its high specific energy, low potential and large storage capacity. However, interfacial problems between argyrodite SSEs and the anode (interfacial reactions, lithium dendrites, etc.) are considered to be important factors affecting their availability. In this mini review, we summarize the behavior, properties and problems arising at the interface between argyrodite SSEs and anode. Strategies to solve interface problems and stabilize interfaces in recent years are also discussed. Finally, a brief outlook about argyrodite SSEs is presented.