Breaking the boundaries of Li-S batteries with high-entropy engineered multifunctional materials

Abstract

Lithium-sulfur (Li-S) batteries promise exceptional theoretical energy density but face persistent challenges, notably polysulfide shuttling and sluggish redox kinetics. High-entropy materials (HEMs), leveraging their distinctive configurational entropy and unparalleled compositional tunability, offer a transformative approach to engineer electrochemical interfaces and address these critical limitations. This review comprehensively surveys the recent advancements in the rational design and application of HEMs for Li-S batteries. We first analyze the structural and electronic characteristics of HEMs and clarify how they enhance sulfur utilization, suppress lithium polysulfides (LiPSs) shuttling by anchoring intermediates, and accelerate LiPSs redox reactions through tailored electronic structures. Subsequently, state-of-the-art design strategies are critically examined, including atomic-scale elemental selection, advanced synthetic methodologies, and multidimensional structural engineering. These strategies enable fabrication of components such as sulfur hosts with optimized adsorption and catalytic sites, separator modifiers that regulate ion-selective transport, and protective interlayers that mitigate lithium dendrite growth. Furthermore, we systematically review cutting-edge characterization techniques and computational methods that detail the mechanisms behind entropy-mediated improvements in battery performance. Finally, critical challenges and promising future research directions are highlighted for the development of next-generation HEM-based energy storage systems, and the insights presented in this review will guide the rational design and practical implementation of HEMs in advanced Li-S batteries.