Orchestrating Penta‐Element Interplay in Gradient‐Porous Carbons for Advanced Sodium‐Ion Hybrid Capacitors
Yangjie Liu, Yao Guo, Yu Zhang, Lihong Xu, Junxiang Chen, Xiang Hu, Zhenhai Wen
Abstract
Abstract Sodium‐ion hybrid capacitors (SIHCs) offer a cutting‐edge synergy between battery‐level energy density and supercapacitor‐like power density, yet face critical challenges in balancing the kinetic and capacity mismatch between Faradaic anodes and capacitive cathodes. Herein, we present a penta‐element doped gradient‐porous carbon (PE‐GPC) with a nanosphere architecture, engineered with high‐entropy principles and a gradual pore density variation to enhance mass transport and charge storage. Operando spectroscopy and machine learning potentials unveil a concerted penta‐element interplay: thiophene‐like S configurations mediate dynamic redox processes, enabling pseudocapacitive Na⁺ and anion storage, while fluorine functionalities foster a self‐rejuvenating NaF‐rich solid electrolyte interphase (SEI), stabilizing long‐term cycling. Meanwhile, the synergistic N/B/P triad engineers a hierarchical defect network that enhances electronic conductivity and fine‐tunes ion adsorption energetics. This orchestrated interplay empowers the SIHC full cell with a high energy density of 196 Wh kg −1 , a formidable power density (10.4 kW kg −1 ), and an impressive 88.2% capacity retention after 9000 cycles. By establishing a high‐entropy stabilization paradigm, this work paves the way for multi‐ion storage architectures, offering a universal strategy to bridge the charge‐transfer imbalance in advanced energy devices.