“Electronic Highway” and “Heterometal Seed” in Stable Ag‐N/P Coordination for High‐Performance Aqueous Zinc Ion Hybrid Capacitors

Abstract With the rapid development of electrochemical energy storage technology, aqueous zinc‐ion hybrid capacitors (AZICs) have emerged as a promising energy storage systems due to their high safety, low cost, and environmental friendliness. Metal nanoparticles (NPs) (e.g., Ag) incorporated carbon‐based materials, as cathode materials for AZICs, exhibit promising electrochemical properties. However, metallic Ag atoms exhibit extremely high surface energy, which induces aggregation, leading to rapid capacity degradation. In this study, Ag NPs‐anchored N/P co‐doped porous carbon cathode (Ag@NPC) is designed and fabricated. DFT calculations show that P orbital that facilitates electron delocalization, can interconnect with electron accumulation around N atoms obtained from Ag NPs to create a highly delocalized electronic system for Ag‐C stable interfacial interaction and rapid Zn 2+ transmission. Ag NPs undergo reversible Ag/Ag 2 SO 4 redox reactions and serve as “heterometal seeds” facilitating Zn 2+ uniform nucleation. Experimental results demonstrate that the Ag@NPC cathode exhibits a high specific capacity of 239 mAh g −1 at 0.1 A g −1 , outstanding capacity retention of 91.1% after 20 000 cycles, a high energy density of 161.2 Wh kg −1 , and remarkable anti‐self‐discharge performance. This work offers new insights for the design of high‐performance metal‐carbon composite materials and sustainable energy storage systems.