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Sulfide solid electrolytes (SSEs) have garnered significant attention for their high ionic conductivity in the development of all‐solid‐state batteries (ASSBs). However, SSEs face challenges due to poor chemical and electrochemical stability, leading to SE decomposition at the anode, which in turn increases internal resistance and reduces cycle performance. Herein, to address this issue, thin polymer layers are applied to prevent direct contact between the SSE and anode using the initiated chemical vapor deposition process. This method facilitates the uniform coating of eight types of polymers with polar functionalities on indium (In) anodes. Half‐cell tests and X‐ray photoelectron spectroscopy analysis reveals that poly(acrylic acid) and poly((perfluorohexyl)ethyl acrylate), containing ─COOH and C─F bonds respectively, effectively stabilized the In/SSE interface. In full cells assembled with polymer‐coated In and LiNi0.8Co0.1Mn0.1O2 (NCM811), capacity retention show remarkable improvement, achieving 64.8% for In@pAA and 50.7% for In@pC6FA after 100 cycles, compared to 29.0% for bare In. This study provides insights into the interaction between polar bonds in polymers and SSEs, potentially bridging a significant knowledge gap resulting from the significant lack of research investigating the relationship between polymers, one of the primary materials commonly used in ASSBs. [ABSTRACT FROM AUTHOR]

All‐solid‐state batteries (SSBs) represent one of the most promising avenues for surpassing the energy density limitations of conventional lithium‐ion batteries. However, the unstable interfacial contact between the solid‐state electrolyte and the electrode poses a critical challenge for practical applications. To tackle this issue, a hybrid system incorporating both liquid electrolytes (LEs) and sulfide solid‐state electrolytes may serve as a viable alternative. In this hybrid system, the LE facilitates the in situ formation of a solid electrolyte interphase layer, thereby enhancing the physical interface contact. Consequently, the electrochemical lifetime of the hybrid all‐SSBs is significantly improved, as evidenced by the stable lithium plating behavior observed through analytical techniques such as in situ X‐ray imaging. Nonetheless, the hybrid system exhibits clear limitations, and several issues that need to be addressed for its practical implementation are identified. In conclusion, potential solutions that could be employed to overcome these challenges are proposed. [ABSTRACT FROM AUTHOR]

Anode‐free Li metal batteries are one of the finest prospects for increasing energy density beyond that of standard lithium‐ion batteries. Conversely, the absence of Li reservoir generates unwarranted volume expansion, permitting electrolyte depletion and rapid cathode capacity consumption. To address this issue, an anode‐free Li metal battery with an ion‐conductive layer coated Cu current collector Ag/L in typical carbonate‐based electrolytes is presented. The ion‐conducting layer causes stable solid electrolyte interphase development and allows for minimal volume expansion when utilizing stable Li hosts. Via density functional theory calculation and experimental measurements and analysis, the beneficial effect of Li hosting behavior of the ion‐conductive layer is demonstrated. Furthermore, anode‐free electrochemical performance with high discharge capacity retention, which is exceptional in a traditional carbonate electrolyte with LiNi0.8Mn0.1Co0.1O2 based cathode (4.2 mAh cm−2) and high current density (2.1 mA cm−2) is shown. To prove material compatibility, argyrodite sulfide solid electrolytes instead of liquid electrolytes, which show Coulombic efficiency of 97% at 50 cycles in all‐solid‐state Li half‐cells are used. [ABSTRACT FROM AUTHOR]

Rechargeable batteries have been a profoundly greater part of our lives than we could have ever imagined. The rechargeable Li‐ion batteries (LIBs) that have been developed for transport systems even put fossil fuels in the corner. However, state‐of‐the‐art Li‐ion batteries with graphite anodes are now approaching their theoretical specific energy limits, so they cannot meet the increasing demands of a range of portable electronics and large‐scale energy storage systems. Li metal is one of the most promising anode materials that could break through the energy density bottleneck of Li‐ion batteries due to its ultrahigh specific capacity and very low potential compared to other anode materials. Nonetheless, the direct use of Li metal in commercial battery systems has been hindered due to significant obstacles associated with it such as safety issues, corrosion from chemical reactions that occur inside the battery, or poor cycling performance. The fundamental reason for these problems is the dendritic growth of Li‐ions on the Li metal anode during cycling, as a result of the interfacial phenomena of Li metal and electrolytes. Modification of the Li metal interface with an electrolyte presents an efficient solution to solve these problems. In this review, the current challenges facing the development of Li metal anodes are presented in detail. The most recent advances in Li metal anodes using a controlled interface between the Li metal surface and an electrolyte are highlighted and an introduction on the synthesis and production methods for the application of high‐energy‐density battery systems such as Li‐oxygen (Li−O2), Li‐sulfur (Li−S), and Li metal batteries with high‐energy density cathodes is presented. Furthermore, the recent developments in the in situ/operando analysis tools adopted for the investigation of Li metal anodes such as the structural and chemical changes, dynamic properties, and solid–electrolyte interface (SEI) layer properties are described and summarized. Finally, some suggestions are given in the direction of the development of Li metal with artificial surface layers for use in future high‐energy batteries. [ABSTRACT FROM AUTHOR]