Ultrathin Nitrogen‐Doped Carbon Layer Uniformly Supported on Graphene Frameworks as Ultrahigh‐Capacity Anode for Lithium‐Ion Full Battery

Abstract The designable structure with 3D structure, ultrathin 2D nanosheets, and heteroatom doping are considered as highly promising routes to improve the electrochemical performance of carbon materials as anodes for lithium‐ion batteries. However, it remains a significant challenge to efficiently integrate 3D interconnected porous frameworks with 2D tunable heteroatom‐doped ultrathin carbon layers to further boost the performance. Herein, a novel nanostructure consisting of a uniform ultrathin N‐doped carbon layer in situ coated on a 3D graphene framework (NC@GF) through solvothermal self‐assembly/polymerization and pyrolysis is reported. The NC@GF with the nanosheets thickness of 4.0 nm and N content of 4.13 at% exhibits an ultrahigh reversible capacity of 2018 mA h g −1 at 0.5 A g −1 and an ultrafast charge–discharge feature with a remarkable capacity of 340 mA h g −1 at an ultrahigh current density of 40 A g −1 and a superlong cycle life with a capacity retention of 93% after 10 000 cycles at 40 A g −1 . More importantly, when coupled with LiFePO 4 cathode, the fabricated lithium‐ion full cells also exhibit high capacity and excellent rate and cycling performances, highlighting the practicability of this NC@GF.