Cascade Desolvation and Conversion Reaction Driven by Self‐Tandem Catalysis for Wide‐Temperature Li‐S Batteries

Dissatisfactory electrochemical performance of wide‐temperature lithium‐sulfur batteries (LSBs) originates from the sluggish Li + desolvation and successive sulfur specie conversion kinetics at the interface and within the cathode interior. Herein, different from electrolyte engineering, a self‐tandem catalysis enabled cascade reactions is developed to drive Li + kinetics and associated polysulfide conversions in wide‐temperature LSBs. By incorporating electron‐adjustable atom‐level Ce as the self‐tandem catalyst onto defect‐rich Co, Fe‐based layered double hydroxides (EAAC@D‐LDH), a favorable solvation microenvironment is established to decrease the related barriers toward promoting rapid Li + desolvation, sulfur conversion, and Li 2 S delithiation kinetics, as revealed in Raman analysis, electrochemical evaluations, and ex‐situ interfacial morphology as well as composition characterization. Such improved reaction kinetics enable the sulfur cathodes work well in a wide temperature ranging from 0 to ‐30°C, and it retains high‐capacity retention of 94% at 5C. Under ‐20°C, the cells remain the capacity of 85% at 0.1C, respectively. Remarkably, a stable capacity is reserved even at an ultralow temperature of ‐30°C, demonstrating that the substantial promise of this self‐tandem catalysis supports cascade reaction refinement strategy toward high performance wide‐temperature LSBs.