Supramolecular‐Derived Heterostructured Carbon Supported with Mo Single Atoms for High‐Capacity and Long‐Cycle Sodium Dual‐Ion Batteries

ABSTRACT Owing to their inherent advantages of high operating voltage, low cost, and environmental friendliness, all‐carbon sodium dual‐ion batteries (SDIBs) are highly competitive in the post‐lithium era and hold great promise for large‐scale energy storage. The long‐range ordered graphitized carbon and amorphous non‐graphitized carbon exhibit distinct Na + storage behavior due to their fundamentally different structural configurations. While the diverse structures and physicochemical properties of supramolecular precursors offer a novel approach for the construction of heterostructured carbon with superior performance, which can integrate the respective advantages of graphitized and non‐graphitized carbon to achieve multifunctionality. Moreover, single atoms supported on the carbon matrix can further enhance the kinetic properties, promote ion/electron transport, and accelerate the redox conversion. Herein, supramolecular‐derived nitrogen‐doped heterostructured carbon (Mo‐NHC) supported with Mo single atoms is synthesized and demonstrates a breakthrough achievement for carbonaceous materials in Na + storage. Proof‐of‐concept SDIBs exhibit a high discharge capacity of 222.3 mA h g −1 with a retention of 80.4% after 10,000 cycles. Even under high mass loading and high‐temperature conditions, it still achieves extraordinary reversible capacity and cyclic stability. This work represents one of the best performances among all‐carbon SDIBs, providing an advanced material paradigm for heterostructured carbon in electrochemical energy storage.