Bimetallic Coupling Strategy Modulating Electronic Construction to Accelerate Sulfur Redox Reaction Kinetics for High‐Energy Flexible Li‐S Batteries

Abstract Lithium‐sulfur (Li‐S) batteries are considered the most promising energy storage battery due to their low cost and high theoretical energy density. However, the low utilization rate of sulfur and slow redox kinetics have seriously limited the development of Li‐S batteries. Herein, the electronic state modulation of metal selenides induced by the bi‐metallic coupling strategy is reported to enhance the redox reaction kinetics and sulfur utilization, thereby improving the electrochemical performance of Li‐S batteries. Theoretical calculations reveal that the electronic structure can be modulated by Ni‐Co coupling, thus lowering the conversion barrier of lithium polysulfides (LiPSs) and Li + , and the synergistic interaction between NiCoSe nanoparticles and nitrogen‐doped porous carbon (NPC) is facilitating to enhance electron transport and ion transfer kinetics of the NiCoSe@NPC‐S electrodes. As a result, the assembled Li‐S batteries based on NiCoSe@NPC‐S exhibit high capacities (1020 mAh g −1 at 1 C) and stable cycle performance (80.37% capacity retention after 500 cycles). The special structural design and bimetallic coupling strategy promote the batteries working even under lean electrolyte (7.2 µL mg −1 ) with a high sulfur loading (6.5 mg cm −2 ). The proposed bimetallic coupling strategy modulating electronic construction with N‐doping porous carbon has jointly contributed the good redox reaction kinetics and high sulfur utilization.