Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector. Four types of ion-conducting, inorganic solid electrolytes are tested: Amorphous 70/30 mol% Li2S-P2S5, polycrystalline β-Li3PS4, and polycrystalline and single-crystalline Li6La3ZrTaO12 garnet. The nature of lithium plating depends on the proximity of the current collector to defects such as surface cracks and on the current density. Lithium plating penetrates/infiltrates at defects, but only above a critical current density. Eventually, infiltration results in a short circuit between the current collector and the Li-source (anode). These results do not depend on the electrolytes shear modulus and are thus not consistent with the Monroe–Newman model for “dendrites.” The observations suggest that Li-plating in pre-existing flaws produces crack-tip stresses which drive crack propagation, and an electrochemomechanical model of plating-induced Li infiltration is proposed. Lithium short-circuits through solid electrolytes occurs through a fundamentally different process than through liquid electrolytes. The onset of Li infiltration depends on solid-state electrolyte surface morphology, in particular the defect size and density.

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Solid-state batteries (SSBs) are considered as one of the most promising candidates for the next-generation energy-storage technology, because they simultaneously exhibit high safety, high energy density, and wide operating temperature range. The replacement of liquid electrolytes with solid electrolytes produces numerous solid-solid interfaces within the SSBs. A thorough understanding on the roles of these interfaces is indispensable for the rational performance optimization. In this Review, we discuss the interface issues in the SSBs, including internal buried interfaces within solid electrolytes and composite electrodes, and planar interfaces between electrodes and solid electrolyte separators or current collectors. The challenges and future directions on the investigation and optimization of these solid-solid interfaces for the production of the SSBs are also assessed. This article is protected by copyright. All rights reserved.

Role of Interfaces in Solid-State Batteries.

Over the past few years, halide solid-state electrolytes (HSSEs) have attracted the attention of researchers, and many reports about HSSEs have been published. Their wide electrochemical window (ECW) and a quite good compatibility with the popular oxide cathode materials make them attractive for practical applications. As a result, HSSEs are exciting candidates for the future generation of all-solid-state Li batteries (ASSLBs). In recent years, noticeable efforts have been made to develop novel HSSEs and utilize them in ASSLBs. Herein, a comprehensive update on the progress of HSSEs development and their application in ASSLBs is provided. First, a brief summary of the conductivity of HSSEs and potential synthesis approaches is provided. Next, the moisture and phase stabilities of HSSEs are reviewed separately, and the techniques proposed in the recently published reports to achieve sufficient stabilities are summarized. In addition, the electrochemical stabilities of HSSEs with Li metal anode and oxide cathode materials, from experimental and theoretical points of view, are provided in parallel. Furthermore, the application and progress of HSSEs in high-voltage ASSLBs are discussed. Finally, new research directions are suggested for the development of scalable HSSEs-based ASSLBs. 

Halide Solid‐State Electrolytes: Stability and Application for High Voltage All‐Solid‐State Li Batteries

Lithium nitrate is widely used as an additive in electrolytes to regulate the solid electrolyte interphase (SEI). However, the application of LiNO3 in lithium metal batteries (LMBs) is limited by its extremely low solubility in conventional carbonate‐based electrolytes. In this study, a non‐flammable deep eutectic solvent (DES) with lithium bis(trifluoromethanesulfonyl)imide and N‐methylacetamide (NMAC) as the main components is chosen as the LMB electrolyte. Using theoretical calculations and experiments, the strong interaction between NMAC and LiNO3 is proved to be effective in increasing the solubility of LiNO3 (up to 4 wt%) and realizing stable anion‐rich SEI layers. DES synergizes with LiNO3 to produce LiF, LixN, and LiNxOy enriched SEI layer, which improves the uniformity of lithium deposition. In particular, the NCM622||DES‐2||Li full cells achieve 84% capacity retention after 600 cycles at 0.5 C, far exceeding that of conventional carbonate electrolytes (56%). Consequently, this study provides a new strategy for employing LiNO3 in LMBs, in addition to its potential application in other alkali metal batteries and anode‐free batteries.

Highly Stable Lithium Metal Batteries by Regulating the Lithium Nitrate Chemistry with a Modified Eutectic Electrolyte

In recent years, solid-state lithium batteries (SSLBs) using solid electrolytes (SEs) have been widely recognized as the key next-generation energy storage technology due to its high safety, high energy density, long cycle life, good rate performance and wide operating temperature range. However, SSLBs still suffer from many obstacles that hinder their practical application. This review discusses typical lithium-ion conductors and their in-depth lithium-ion conduction mechanism. The key interfacial problems of electrolytes and electrodes for SSLBs are comprehensively elaborated and several possible solution methods are proposed. Furthermore, three viable manufacturing strategies for free-standing thin SE membranes are discussed in details. Moreover, for the first time, the government policies and latest company industrialization process relative to SSLBs worldwide are systematically summarized. Finally, several potential strategies are identified for the future development of high-energy-density SSLBs. 

Solid-State Lithium Batteries-From Fundamental Research to Industrial Progress

Stable all-solid-state lithium metal batteries with Li3N-LiF-enriched interface induced by lithium nitrate addition

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Stable all-solid-state lithium metal batteries with Li3N-LiF-enriched interface induced by lithium nitrate addition