Critical Challenges and Optimization Strategies for Rechargeable Aluminum‐Sulfur Batteries

Abstract The increasing demand for efficient, cost‐effective energy storage systems has spurred research into alternatives to lithium‐ion batteries. Among these alternatives, aluminum‐sulfur (Al‐S) batteries have become a promising option, demonstrating noteworthy advancements over the past decade. These batteries provide benefits such as high theoretical energy density, low cost, and improved safety. Nonetheless, certain fundamental electrochemical challenges, similar to those encountered by other sulfur‐based batteries, persist, including slow reaction kinetics, significant polysulfide shuttling, and uncontrollable dendrite growth on the anode. Herein, this review offers a comprehensive overview of recent advancements related to the critical challenges and optimization strategies for rechargeable Al‐S batteries. It begins by outlining the development history of Al‐S batteries and the challenges present in current systems. Next, efficient optimization strategies aimed at enhancing Al‐S batteries are summarized by focusing on optimizing each battery component, including the cathode, anode, electrolyte, and separator. Detailed examinations include structural features, electrochemical performance, structure‐property correlations, and enhancement mechanisms of key breakthroughs. Finally, the challenges and potential opportunities are explored for future research on rechargeable Al‐S batteries. This review aims to provide insightful guidance for the rational design of high‐performance Al‐S batteries and to accelerate their development for practical large‐scale energy storage applications.