Tailoring the Li+ Intercalation Energy of Carbon Nanocage Anodes Via Atomic Al‐Doping for High‐Performance Lithium‐Ion Batteries

Abstract Graphitic carbon materials are widely used in lithium‐ion batteries (LIBs) due to their stability and high conductivity. However, graphite anodes have low specific capacity and degrade over time, limiting their application. To meet advanced energy storage needs, high‐performance graphitic carbon materials are required. Enhancing the electrochemical performance of carbon materials can be achieved through boron and nitrogen doping and incorporating 3D structures such as carbon nanocages (CNCs). In this study, aluminum (Al) is introduced into CNC lattices via chemical vapor deposition (CVD). The hollow structure of CNCs enables fast electrolyte penetration. Density functional theory (DFT) calculations show that Al doping lowers the intercalation energy of Li + . The Al–boron (B)–nitrogen (N‐doped CNC (AlBN‐CNC) anode demonstrates an ultrahigh rate capacity (≈300 mAh g −1 at 10 A g −1 ) and a prolonged fast‐charging lifespan (862.82 mAh g −1 at 5 A g −1 after 1000 cycles), surpassing the N‐doped or BN‐doped CNCs. Al doping improves charging kinetics and structural stability. Surprisingly, AlBN‐CNCs exhibit increased capacity upon cycling due to enlarged graphitic interlayer spacing. Characterization of graphitic nanostructures confirms that Al doping effectively tailors and enhances their electrochemical properties, providing a new strategy for high‐capacity, fast‐charging graphitic carbon anode materials for next‐generation LIBs.