N‐Doping and Defective Nanographitic Domain Coupled Hard Carbon Nanoshells for High Performance Lithium/Sodium Storage

Hard carbons (HCs) possess high lithium/sodium storage capacities, which however suffer from low electric conductivity and poor ion diffusion kinetics. An efficient structure design with appropriate heteroatoms doping and optimized graphitic/defective degree is highly desired to tackle these problems. This work reports a new design of N‐doped HC nanoshells (N‐GCNs) with homogeneous defective nanographite domains, fabricated through the prechelation between Ni²⁺ and chitosan and subsequent catalyst confined graphitization. The as‐prepared N‐GCNs deliver a high reversible lithium storage capacity of 1253 mA h g^?1, with outstanding rate performance (175 mA h g^?1 at a high rate of 20 A g^?1) and good cycling stability, which outperforms most state‐of‐the‐art HCs. Meanwhile, a high reversible sodium storage capacity of 325 mA h g^?1 is also obtained, which stabilizes at 174 mA h g^?1 after 200 cycles. Density functional theory calculations are performed to uncover the coupling effect between heteroatom‐doping and the defective nanographitic domains down to the atomic scale. The in situ Raman analysis reveals the “adsorption mechanism” for sodium storage and the “adsorption–intercalation mechanism” for lithium storage of N‐GCNs.