Co/CoS Heterojunction Embedded in N, S-Doped Hollow Nanocage for Enhanced Polysulfides Conversion in High-Performance Lithium-Sulfur Batteries.

Modulating the electronic configuration of the substrate to achieve the optimal chemisorption toward polysulfides (LiPSs) for boosting polysulfide conversion is a promising way to the efficient Li-S batteries but filled with challenges. Herein, a Co/CoS heterostructure is elaborately built to tuning d-orbital electronic structure of CoS for a high-performance electrocatalyst. Theoretical simulations first evidence that Co metal as the electron donator can form a built-in electric field with CoS and downshift the d-band center, leading to the well-optimized adsorption strength for lithium polysulfides on CoS , thus contributing a favorable way for expediting the redox reaction kinetics of LiPSs. As verification of prediction, a Co/CoS heterostructure implanted in porous hollow N, S co-doped carbon nanocage (Co/CoS @NSC) is designed to realize the electronic configuration regulation and promote the electrochemical performance. Consequently, the batteries assembled with Co/CoS @NSC cathode display an outstanding specific capacity and an admirable cycling property as well as a salient property of 8.25 mAh cm under 8.18 mg cm . The DFT calculation also reveals the synergistic effect of N, S co-doping for enhancing polysulfide adsorption as well as the detriment of excessive sulfur doping.