Ultrahigh Pyridinic/Pyrrolic N Enabling N/S Co‐Doped Holey Graphene with Accelerated Kinetics for Alkali‐Ion Batteries

Carbonaceous materials hold great promise for K-ion batteries due to their low cost, adjustable interlayer spacing, and high electronic conductivity. Nevertheless, the narrow interlayer spacing significantly restricts their potassium storage ability. Herein, hierarchical N, S co-doped exfoliated holey graphene (NSEHG) with ultrahigh pyridinic/pyrrolic N (90.6 at.%) and large interlayer spacing (0.423 nm) is prepared through micro-explosion assisted thermal exfoliation of graphene oxide (GO). The underlying mechanism of the micro-explosive exfoliation of GO is revealed. The NSEHG electrode delivers a remarkable reversible capacity (621 mAh g^-1 at 0.05 A g^-1), outstanding rate capability (155 mAh g^-1 at 10 A g^-1), and robust cyclic stability (0.005% decay per cycle after 4400 cycles at 5 A g^-1), exceeding most of the previously reported graphene anodes in K-ion batteries. In addition, the NSEHG electrode exhibits encouraging performances as anodes for Li-/Na-ion batteries. Furthermore, the assembled activated carbon||NSEHG potassium-ion hybrid capacitor can deliver an impressive energy density of 141 Wh kg^-1 and stable cycling performance with 96.1% capacitance retention after 4000 cycles at 1 A g^-1. This work can offer helpful fundamental insights into design and scalable fabrication of high-performance graphene anodes for alkali metal ion batteries.