Orchestrating Penta-Element Interplay in Gradient-porous Carbons for Advanced Sodium-Ion Hybrid Capacitors.

Journal: Angewandte Chemie (International ed. in English)
Published Date: Jun 24, 2025

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.

Authors

  • Yangjie Liu
    Chinese Academy of Sciences Fujian Institute of Research on the Structure of Matter, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research, on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002,, CHINA.
  • Yao Guo
  • Yu Zhang
    College of Marine Electrical Engineering, Dalian Maritime University, Dalian, China.
  • Lihong Xu
    Department of Control Science and Engineering, Tongji University, Shanghai 201804, China.
  • Junxiang Chen
    School of Medicine, University of Pittsburgh, Pittsburgh, PA, United States.
  • Xiang Hu
    Department of Endocrinology and Metabolism, Shanghai Jiao Tong University Affiliated Sixth People's Hospital, Shanghai Clinical Center for Diabetes, Shanghai Key Laboratory of Diabetes Mellitus, Shanghai Diabetes Institute Shanghai 200233, China.
  • Zhenhai Wen
    Fujian Institute of Research on the Structure of Matter, Chinese Academy of Science, Institute of Materials, 155 Yangqiao Road West, 350002, Fuzhou, CHINA.

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