Rational Designing MxSy@C (M=Ni, Co, Zn, Cu, Mn) Composites with Controlled Polysuifides Shuttling Behaviors towards Advanced Stable Room Temperature Na‐S Batteries†

Comprehensive Summary Room‐temperature sodium‐sulfur (RT‐Na/S) batteries display attractive potential in large‐scale energy‐storage, but their practical application was still restricted by the serious dissolution of polysulfides. Herein, supported by the constructing of interface engineering, the metal sulfide‐carbon nanocomposite can be prepared with considerable electrochemical properties. Utilizing the double‐helix structure of carrageenan‐metal hydrogels as precursors, in‐situ metal sulfide (M x S y ) nanostructure/3D carbon aerogels (3D CAs) can be successfully constructed. Importantly, with the assistance of the vulcanization process, 3D carbon architecture was maintained in the composites and acted as a skeleton to optimize their structural stability. As the cathode of RT‐Na/S batteries, ZnS/S@C and NiS 2 /S@C delivered an excellent cycling stability and rate performance (179.8 mAh·g −1 at 20 A·g −1 after 10000 cycling for ZnS/S@C, 220.3 mAh·g −1 at 10 A·g −1 after 3000 cycling for NiS 2 /S@C). The detailed investigation of mechanism revealed that the powerful adsorption for Na 2 S 4 originated from 3D metal sulfide‐carbon structure. The well‐designed architecture of sulfide‐carbon composites servers as an electrocatalyst to alleviate the shuttle effect of polysulfides, resulting in the long‐term electrochemical stability. Given this, the work is expected to provide promising insights for designing advanced cathode materials for RT‐Na/S batteries.