Multidimensional Integrated Chalcogenides Nanoarchitecture Achieves Highly Stable and Ultrafast Potassium‐Ion Storage

Potassium‐ion batteries (KIBs) have come into the spotlight in large‐scale energy storage systems because of cost‐effective and abundant potassium resources. However, the poor rate performance and problematic cycle life of existing electrode materials are the main bottlenecks to future potential applications. Here, the first example of preparing 3D hierarchical nanoboxes multidimensionally assembled from interlayer‐expanded nano‐2D MoS2@dot‐like Co9S8 embedded into a nitrogen and sulfur codoped porous carbon matrix (Co9S8/NSC@MoS2@NSC) for greatly boosting the electrochemical properties of KIBs in terms of reversible capacity, rate capability, and cycling lifespan, is reported. Benefiting from the synergistic effects, Co9S8/NSC@MoS2@NSC manifest a very high reversible capacity of 403 mAh g−1 at 100 mA g−1 after 100 cycles, an unprecedented rate capability of 141 mAh g−1 at 3000 mA g−1 over 800 cycles, and a negligible capacity decay of 0.02% cycle−1, boosting promising applications in high‐performance KIBs. Density functional theory calculations demonstrate that Co9S8/NSC@MoS2@NSC nanoboxes have large adsorption energy and low diffusion barriers during K‐ion storage reactions, implying fast K‐ion diffusion capability. This work may enlighten the design and construction of advanced electrode materials combined with strong chemical bonding and integrated functional advantages for future large‐scale stationary energy storage. The first example of preparing 3D hierarchical nanoboxes multidimensionally assembled from interlayer‐expanded nano‐2D MoS2@dot‐like Co9S8 embedded into a nitrogen and sulfur codoped porous carbon matrix (Co9S8/NSC@MoS2@NSC) for greatly boosting the electrochemical properties of potassium‐ion batteries in terms of reversible capacity, rate capability, and cycling stability, is reported.