Anion‐Vacancy Modified WSSe Nanosheets on 3D Cross‐Networked Porous Carbon Skeleton for Non‐Aqueous Sodium‐Based Dual‐Ion Storage

Abstract Sodium‐based dual‐ion batteries (SDIBs) have become a new type of energy storage device with great application value because of their high operating voltage, high energy density, and low cost. However, transition‐metal dichalcogenide (TMD) anodes show unsatisfactory Na + electrochemical performance owing to the low intrinsic conductivity and inferior ion transport kinetics. Here, an elaborate design is developed to prepare a composite of WSSe nanosheets supported on a 3D cross‐networked porous carbon skeleton (WSSe@CPCS), which possesses en‐rich anion vacancies and WSSe with expanded inter‐layer spacing, as well as an interconnected porous structure. As a result, the WSSe@CPCS anode for sodium‐ion batteries (SIBs) exhibits preeminent reversible capacities, excellent cycle stability, and superior rate capability. The systematic electrochemical kinetic analysis and density functional theory results further show that the effect of anion vacancies and CPCS synergistically enhances the conductivity and reduces charge transfer resistance, thus making a great contribution to fast reaction kinetics. Finally, the implementations of the WSSe@CPCS anode in progressive SIB and DIB full‐cell configurations exhibit satisfactory performance, which reveals their widely practical application. This research will provide an exciting approach to designing advanced defect‐structured tungsten‐based TMD materials for SIBs, DIBs, and even a broad range of energy storage.