Enhanced Kinetics Harvested in Heteroatom Dual‐Doped Graphitic Hollow Architectures toward High Rate Printable Potassium‐Ion Batteries

Abstract Carbonaceous materials have emerged as promising anode candidates for potassium‐ion batteries (PIBs) due to overwhelming advantages including cost‐effectiveness and wide availability of materials. However, further development in this realm is handicapped by the deficiency in their in‐target and large‐scale synthesis, as well as their low specific capacity and huge volume expansion. Herein the precise and scalable synthesis of N/S dual‐doped graphitic hollow architectures (NSG) via direct plasma enhanced chemical vapor deposition is reported. Thus‐fabricated NSG affording uniform nitrogen/sulfur co‐doping, possesses ample potassiophilic surface moieties, effective electron/ion‐transport pathways, and high structural stability, which bestow it with high rate capability (≈100 mAh g −1 at 20 A g −1 ) and a prolonged cycle life (a capacity retention rate of 90.2% at 5 A g −1 after 5000 cycles), important steps toward high‐performance K‐ion storage. The enhanced kinetics of the NSG anode are systematically probed by theoretical simulations combined with operando Raman spectroscopy, ex situ X‐ray photoelectron spectroscopy, and galvanostatic intermittent titration technique measurements. In further contexts, printed NSG electrodes with tunable mass loading (1.84, 3.64, and 5.65 mg cm −2 ) are realized to showcase high areal capacities. This study demonstrates the construction of a printable carbon‐based PIB anode, that holds great promise for next‐generation grid‐scale PIB applications.