Engineering Local Graphitic Domains to Balance Defect Active Site and Electronic Conduction Ability in Coal‐Derived Carbon Anode for Superior Potassium Ions Storage

Abstract Potassium‐ion hybrid capacitors (PIHCs) are regarded as one of the promising candidates for large‐scale energy storage technologies. Nevertheless, the lack of suitable anode materials combined with fast ion diffusion kinetics and favorable cycle stability restricts their application. Herein, a catalyst‐confined graphitization strategy is proposed to synthesize low‐cost coal‐based carbon anodes, which have controllable heteroatom co‐doping and rich defect sites, together with local graphitic domains. Density functional theory calculations and kinetic analysis are performed to uncover the coupling effect for heteroatom dual‐doping and defective structures. Importantly, the introduction of graphitic domains ensures good electric conductivity and charge transfer kinetics while preserving rich defects and active sites. The optimized NC‐950 exhibits superior potassium storage capacity, which delivers a high reversible specific capacity (363.3 mAh g⁻¹), impressive rate capability (93.9 mAh g⁻¹ at 2 A g⁻¹), and stable cycling performance. As a practical device application, the PIHCs (NC‐950//AC) are assembled using the NC‐950 anode and commercial activated carbon (AC) cathode, which exhibits the maximum energy density of 97.0 Wh kg⁻¹ and excellent cycling stability (10 000 cycles). Significantly, this work unveils a new pathway to developing low‐cost and fast reaction kinetics carbon anode for advanced electrochemical supercapacitors.