Fabrication of Nitrogen-Containing Micro-Expanding Graphite Composites from Waste Graphite Electrodes for Enhanced...

The large-scale generation of waste graphite not only poses environmental challenges but also provides an opportunity for resource recovery. This study proposes a sustainable strategy that utilizes the graphite cutting waste produced during the production of large graphite electrodes through chemical intercalation, microwave-assisted expansion, and in situ urea nitrogen doping techniques to prepare nitrogen-containing micro-expanded graphite (NMG) composite materials. Structural analysis reveals that the nitrogen-doped amorphous carbon layer formed on the expanded graphite (EG) matrix effectively suppresses excessive expansion while preserving its typical worm-like interlayer morphology and porous structure. XPS confirms successful nitrogen doping with predominant pyridinic-N configuration, introducing abundant defect sites and enhancing lithiophilicity. As an anode for LIBs, NMG delivers an exceptional initial discharge capacity of 1907.5 mAh g^-1 at 20 mA g^-1 and maintains 798.2 mAh g^-1 after 50 cycles, nearly twice that of purified waste graphite (G). Remarkably, after 1000 cycles at 1 A g^-1, it retains 650.4 mAh g^-1 with 89.9% capacity retention, indicating an electrochemical activation process. Kinetic analysis reveals that the superior performance originates from synergistic diffusion-controlled intercalation and surface-dominated pseudocapacitance, with nitrogen-doped defect sites and hierarchical pore architecture promoting rapid ion/electron transport and surface faradaic reactions. This work demonstrates a viable pathway for value-added upcycling of waste graphite while providing insights into designing high-performance anodes through integrated defect engineering and heteroatom doping.