Nitrogen‐Stitched rGO/Graphite Bilayer Anodes for Accelerated Li‐Ion Transport and Interfacial Charge Regulation

ABSTRACT Fast charging of graphite anodes is hindered by sluggish Li + desolvation, high interfacial resistance, and unstable solid electrolyte interphase (SEI) formation. Here, we design a nitrogen‐stitched reduced graphene oxide (rGO) buffer layer that forms a compact and chemically regulated bilayer interface with graphite, enabling accelerated Li + transport. Molecular stitching reconstructs rGO into a constrained, defect‐engineered network with embedded nitrogen sites, reducing excessive surface exposure and stabilizing electron pathways. Electrochemical analyses show that N‐stitched rGO enhances both capacitive Li + pre‐adsorption and diffusion‐controlled kinetics. Galvanostatic intermittent titration technique and distribution of relaxation times measurements reveal more than tenfold higher Li + diffusivity and simultaneous suppression of SEI, charge‐transfer, and bulk transport resistances. In situ Raman spectroscopy identifies a transient Li x N signal, providing direct evidence for a nitrogen‐mediated pre‐interaction step that chemically prepares Li + for rapid intercalation. In situ XRD further confirms uniform LiC 12 → LiC 6 transitions in the stitched bilayer. The dien N‐rGO/graphite electrode delivers superior rate performance and long‐term stability, retaining 97.1% capacity after 500 cycles at 1 C. This work establishes nitrogen stitching as an effective strategy for constructing dynamic interfaces that regulate Li⁺ transport and enable next‐generation fast‐charging graphite anodes.