Interchalcogen effect Promoted Positive-Valence-Conversion sulfur Chemistry for High-Energy aqueous sulfur battery

Sulfur, based on the positive-valence conversion, is promising for constructing high-voltage and high-energy zinc batteries (ZBs) due to its multi-electron transfer process. However, the redox conversion of multivalent S in ZBs is still limited and suffers from low active materials utilization and large charge/discharge polarization with poor reversibility. This study presents significant progress, for the first time, on the catalytic S 0 /S 4+ redox behavior based on the interchalcogen effect in ZBs using single-atom selenium (SA-Se), which greatly facilitates electronic conductivity and improves ion diffusion behavior. Notably, up to 1.52 V and 1.37 V discharge plateaus with an impressive discharge capacity up to 587 mAh g −1 is achieved in Zn‖S batteries. Furthermore, benefiting from the enhanced absorption of soluble products based on the interchalcogen effect, the high-voltage Zn‖S battery exhibits remarkable conversion dynamics, excellent cycling performance, high energy density, and superior areal capacity. This catalytic strategy of positive-valence conversion of sulfur based on the interchalcogen effect represents a significant advancement in constructing future high-voltage sulfur-based batteries.