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Lithium (Li) metal is an ideal anode for high energy-density batteries. During Li plating and stripping, however, dendritic Li growth keeps generating an abundance of irreversible or inactive Li, resulting in severe performance degradation, shortcircuiting, and eventually cell failure. Even if various porous frameworks have received considerable attention to directly store Li metals, achievable reversible and rate capabilities of porous hosts were still hindered by their morphological limitations. Still, open pathways are highly required for homogeneous metallization. For this purpose, herein, enriched cavities to zeolitic imidazolate frameworks are strategically introduced by adapting a hard silica template approach. We found that the migration of Li ions is easily accessible to inner pores and cavities away from the surface during Li plating and stripping. This approach eventually utilizes most internal pores and fully facilitates Li-ion transport, eventually enhancing electrochemistry performances such as long-term cyclability and reversible capacity.

Lithium metal batteries (LMBs) are in the spotlight as a next‐generation battery due to their high theoretical capacity. However, LMBs still suffer from inferior cycle stability owing to dendritic lithium (Li) growth during Li plating and stripping, leading to battery explosion. To solve this problem, solid electrolytes have emerged as a promising candidate by suppressing the dendritic Li growth. Despite numerous efforts, however, many challenges, such as low ionic conductivity, air stability, space charge layer, and contact loss issues, have been encountered. This review aims to provide the current challenges and new insights of solid electrolytes and then explore optimal solutions for next‐generation solid electrolytes.

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For realizing all-solid-state batteries (ASSBs), it is highly desirable to develop a robust solid electrolyte (SE) that has exceptional ionic conductivity and electrochemical stability at room temperature. While argyrodite-type Li 6 PS 5 Cl (LPSCl) SE has garnered attention for its relatively high ionic conductivity (∼3.19 × 10 −3 S cm −1 ), it tends to emit hydrogen sulfide (H 2 S) in the presence of moisture, which can hinder the performance of ASSBs. To address this issue, researchers are exploring approaches that promote structural stability and moisture resistance through elemental doping or substitution. Herein, we suggest using zeolite imidazolate framework-8 as a moisture absorbent in LPSCl without modifying the structure of the SE or the electrode configuration. By incorporating highly ordered porous materials, we demonstrate that ASSBs configured with LPSCl SE display stable cyclability due to effective and long-lasting moisture absorption. This approach not only improves the overall quality of ASSBs but also lays the foundation for developing a moisture-resistant sulfide electrolyte.

Carbon-based frameworks as a metallic lithium (Li) host have been widely developed to overcome the drawbacks associated with bare Li metal anode. Achieving a complete understanding of the growth mechanism of the Li clusters in the carbon host remains controversial, however, and requires determining the factors involved and their clear causes. Herein, we have carried out density functional theory calculations to predict the growth mechanism of Li clusters by employing different heteroatoms (pyridinic N, pyrrolic N, quaternary N, and Co−N4). As a key feature, the Co−N4 affects the Li deposition behavior with axial Li growth on the surfaces of the carbon frameworks, while the other heteroatoms (i.e., nitrogen defects) induce vertical Li growth. By combining theoretical calculations and experiments, this detailed investigation widens the scope of future research on carbon host materials for practical usage of Li metal batteries.

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The demand for high-energy Li batteries is rapidly increasing due to the growing market for electric vehicles and portable electronic devices. Lithium (Li) metal has been considered as an ideal anode for high-energy Li batteries because of its high theoretical capacity (3860 mAh g^-1) and low redox potential (-3.04 V vs. SHE). However, the utilization of Li metal anode is still limited by fundamental problems associated with unavoidable dendritic growth and huge volume changes during cycling. To improve the electrochemical performance of Li metal anode, various strategies have been explored including electrolyte design, interfacial engineering, and structural modifications. One of the most promising approaches is to store Li metal in porous host materials, which can effectively suppress the formation of Li dendrite and volume expansion. Herein, we focus on recent progress in the development of advanced Li metal anodes and suggest research directions and design rules.