Suppression strategies for the polysulfide shuttle effect in electrolyte systems

Abstract

Despite their theoretical high energy density, the commercialization of lithium-sulfur (Li-S) batteries has yet to be realized due to fundamental challenges in sulfur redox chemistry. The persistent limitation originates from the tripartite mechanism involving dissolution, unrestricted migration, and parasitic reactions of lithium polysulfides (LiPS), collectively known as the “shuttle effect”, which severely compromises practical energy density and cycling stability. As the primary ionic conductor mediating these processes, electrolyte engineering demonstrates unique advantages through molecular-level regulation of LiPS solubility, suppression of active material diffusion, and interfacial stabilization. This review presents a systematic analysis of advanced electrolyte design strategies and functional additives, focusing on their dual functions in suppressing LiPS shuttling while maintaining efficient sulfur conversion kinetics. Through systematic categorization of solvation modulation, transport restriction, and anode protection approaches, we critically evaluate their implementation challenges and practical applicability. Building on these analyses, we propose design principles for developing high-performance Li-S electrolytes that achieve optimal balance between shuttle mitigation and electrochemical activity.