Abstract
Lithium-sulfur (Li-S) batteries exhibit high energy density potential but suffer from lithium polysulfide (LPS) shuttling and sluggish conversion kinetics, hindering practical application. Here, a novel approach incorporating out-of-plane single-atom catalysts (SACs) into a tetrathiocine-linked porous organic polymer (POP) framework is introduced. This design enables precise spatial distribution of active metal sites, enhancing interactions with soluble LPSs. The out-of-plane configuration further supports unique coordination motifs, accelerating the transformation of soluble LPSs to solid phases and effectively mitigating the shuttle effect. The resultant Pt-based SAC separator achieves outstanding catalytic efficiency, cycling stability, and capacity retention under high sulfur loading. The findings establish a foundational strategy that integrates advanced molecular design with electrochemical performance, offering a promising avenue for improving the practicality and efficiency of Li-S battery technology.