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The use of all‐solid‐state lithium metal batteries (ASSLMBs) has garnered significant attention as a promising solution for advanced energy storage systems. By employing non‐flammable solid electrolytes in ASSLMBs, their safety profile is enhanced, and the use of lithium metal as the anode allows for higher energy density compared to traditional lithium‐ion batteries. To fully realize the potential of ASSLMBs, solid‐state electrolytes (SSEs) must meet several requirements. These include high ionic conductivity and Li+ transference number, smooth interfacial contact between SSEs and electrodes, low manufacturing cost, excellent electrochemical stability, and effective suppression of dendrite formation. This paper delves into the essential requirements of SSEs to enable the successful implementation of ASSLMBs. Additionally, the representative state‐of‐the‐art examples of SSEs developed in the past 5 years, showcasing the latest advancements in SSE materials and highlighting their unique properties are discussed. Finally, the paper provides an outlook on achieving balanced and improved SSEs for ASSLMBs, addressing failure mechanisms and solutions, highlighting critical challenges such as the reversibility of Li plating/stripping and thermal runaway, advanced characterization techniques, composite SSEs, computational studies, and potential and challenges of ASS lithium–sulfur and lithium–oxygen batteries. With this consideration, balanced and improved SSEs for ASSLMBs can be realized.
The use of all‐solid‐state lithium metal batteries (ASSLMBs) has garnered significant attention as a promising solution for advanced energy storage systems. By employing non‐flammable solid electrolytes in ASSLMBs, their safety profile is enhanced, and the use of lithium metal as the anode allows for higher energy density compared to traditional lithium‐ion batteries. To fully realize the potential of ASSLMBs, solid‐state electrolytes (SSEs) must meet several requirements. These include high ionic conductivity and Li+ transference number, smooth interfacial contact between SSEs and electrodes, low manufacturing cost, excellent electrochemical stability, and effective suppression of dendrite formation. This paper delves into the essential requirements of SSEs to enable the successful implementation of ASSLMBs. Additionally, the representative state‐of‐the‐art examples of SSEs developed in the past 5 years, showcasing the latest advancements in SSE materials and highlighting their unique properties are discussed. Finally, the paper provides an outlook on achieving balanced and improved SSEs for ASSLMBs, addressing failure mechanisms and solutions, highlighting critical challenges such as the reversibility of Li plating/stripping and thermal runaway, advanced characterization techniques, composite SSEs, computational studies, and potential and challenges of ASS lithium–sulfur and lithium–oxygen batteries. With this consideration, balanced and improved SSEs for ASSLMBs can be realized.
All‐solid‐state batteries (ASSBs), configured with solid electrolytes, have received considerable attention as a future energy solution across diverse sectors of modern society. Unlike conventional liquid electrolytes in particular, sulfide solid electrolytes have various advantages, such as high ionic conductivity (>10−3 S cm−1), good ductile properties, and thermal stability. Despite these advantages, the practical application of sulfide solid electrolytes in ASSBs is still limited due to their interfacial instability with commercial cathode materials. Unfortunately, the spontaneous formation of a space charge layer (SCL) at the interface between the cathode material and the solid electrolyte leads to heightened interfacial resistance, obstructing Li+ transport. To address this issue, proper interfacial engineering is still required to facilitate smooth Li+ migration across the interfaces. In this respect, various functional materials have been under exploration as buffer layers, which are intended to suppress the formation of the SCL at these interfaces. Herein, focus is given on the critical significance of these buffer layers between cathode materials and sulfide solid electrolytes in the development of ASSBs. Considering the present limitations, future research directions for next‐generation ASSBs are discussed. These insights are poised to offer valuable guidance for the strategic design and development of highly reliable ASSBs.
Silicon (Si) anode is a promising anode material for all‐solid‐state lithium batteries with ultra‐high theoretical specific capacity and low lithium dendrite risk. However, the inevitable vast volume expansion of Si anode during charge/discharge is recognized as a major limitation preventing its commercial application. Herein, an N, S self‐doped amorphous carbon layer coated on porous micron‐sized Si (p‐mSi@C) is designed to construct an electron/ion conducting network while ensuring structural and interfacial stability. Uneven distribution of von mises stresses during p‐mSi lithiation leads to irregular volume expansion and even fragmentation. Meanwhile, the growth of by‐products at the interface between p‐mSi and electrolyte contact leads to a rapid capacity decay. Compared to p‐mSi anode, p‐mSi@C reduces the risk of fragmentation thanks to the stress‐absorbing effect of amorphous carbon, delivering excellent electrochemical performance (2679.65 mAh g−1 at 0.2 mA cm−2 with initial coulombic efficiency of 84%). More importantly, the chemical failure mechanisms of p‐mSi and p‐mSi@C composite anodes are revealed through structural characterization, chemical analysis, and simulation, which provides the necessary theoretical guidance for practicalization.
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