Entropy Engineering-Modulated D-Band Center of Transition Metal Nitrides for Catalyzing Polysulfide Conversion in Lithium-Sulfur Batteries.

The sluggish sulfur redox kinetics and severe polysulfide shuttle effect seriously restrict the cycling stability and lower the sulfur utilization of lithium-sulfur (Li-S) batteries. Efficient catalytic conversion of polysulfides is deemed a crucial strategy to address these issues, but still suffers from an unclear electronic structure-activity relationship and a limited catalysis performance. Herein, entropy engineering-induced electronic state modulation of metal nitride nanoparticles embedded within hollow N-doped carbon (HNC) polyhedra are theoretically and experimentally constructed as a catalyst to accelerate the redox process of sulfur and suppress polysulfide migration in Li-S batteries.