Hard carbons (HCs) have gained much attention for next-generation
high energy density lithium-ion battery (LIB) anode candidates. However,
voltage hysteresis, low rate capability, and large initial irreversible
capacity severely affect their booming application. Herein, a general
strategy is reported to fabricate heterogeneous atom (N/S/P/Se)-doped
HC anodes with superb rate capability and cyclic stability based on
a three-dimensional (3D) framework and a hierarchical porous structure.
The obtained N-doped hard carbon (NHC) exhibits an excellent rate
capability of 315 mA h g–1 at 10.0 A g–1 and a long-term cyclic stability of 90.3% capacity retention after
1000 cycles at 3 A g–1. Moreover, the as-constructed
pouch cell delivers a high energy density of 483.8 W h kg–1 and fast charging capability. The underlying mechanisms of lithium
storage are illustrated by electrochemical kinetic analysis and theoretical
calculations. It is demonstrated that heteroatom doping imposes significant
effects on adsorption and diffusion for Li+. The versatile
strategy in this work opens an avenue for rational design of advanced
carbonaceous materials with high performance for LIB applications.