Supramolecular-Derived Heterostructured Carbon Supported with Mo Single Atoms for High-Capacity and Long-Cycle Sodium...

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.