Rational design of advanced electrocatalysts based on reactivity descriptors for high-performance lithium-sulfur...

Lithium-sulfur batteries (LSBs) possess ultrahigh theoretical energy densities, making them promising candidates for next-generation energy storage. Nevertheless, their practical deployment is fundamentally constrained by the intrinsic shuttle effect of lithium polysulfides (LiPSs) and the kinetically sluggish sulfur conversion. Recent advancements have highlighted the great significance of catalytic chemistry in mitigating these challenges through LiPS immobilization and the reduction of reaction energy barriers. Despite these great achievements, the rational design of advanced catalysts that satisfy the requirements for practical applications remains a great challenge, necessitating an in-depth mechanistic understanding of the chemical and physical factors governing catalytic performance. Herein, this review focuses on descriptor-based research paradigms and their significant advances in LSBs. Firstly, the fundamental chemistry of sulfur conversion in LSBs and the associated rate-limiting steps are elucidated, followed by a discussion on the mechanisms of catalyst modulation strategies and the establishment of correlations between operational functionality and relevant descriptors. Subsequently, three primary types of descriptors, namely, electronic, thermodynamic and structural descriptors, are delineated, together with the corresponding property-performance relationships. Finally, the development of universal descriptors and mechanistic insights enabled by in situ characterization and computational modeling are highlighted. Moreover, the great potential of artificial intelligence for effective descriptor construction is envisioned, which is expected to facilitate the accurate identification and design of highly active catalysts.