Organosulfur Cathodes in Lithium Metal Batteries: Bridging the Gap between Fundamentals and Practical Applications

Abstract High‐specific energy sulfur‐based cathodes have attracted considerable interest in lithium batteries. Organosulfur cathodes offer inherent advantages of high element abundance and an extended cycling life, aligning with the evolving requirements of future energy storage devices. Over the past decade, research efforts have been devoted to optimizing electrochemical performance through the rich and tunable molecular structures of organosulfur compounds. To further advance the fundamental research and practical application of lithium‐organosulfur batteries, a systematical analysis of the correlation between the molecular structures and electrochemical mechanisms of organosulfur cathodes is imperative. This involves deriving the key parameters at the cell level and investigating the feasibility. In this review, the thermodynamics, reaction processes, and electrochemical kinetics of organosulfur cathodes, grounded in fundamental theories of electrochemistry and materials science are discussed. Expanding the insights, comparisons among elemental sulfur, organosulfur, and n‐type organic cathodes (e.g., carbonyl cathodes) are drawn. The gap between fundamentals and practical applications targeting 500 Wh kg −1 lithium organosulfur batteries is highlighted through energy density calculations and identification of key factors affecting pouch cells. Finally, potential strategies and prospects for the overall design of advanced lithium‐organosulfur batteries are proposed, considering both theoretical foundations and practical implementations.