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Hard carbon anodes face critical challenges in achieving durable solid electrolyte interphase (SEI) and ultrafast ion diffusion to complement capacitive cathodes in sodium-ion hybrid capacitors (SIHCs), despite their low-voltage sodium storage advantages. Herein, we propose a computational-experimental symbiosis resolving this impasse. Density functional theory (DFT) screening reveals that dual fluorine/nitrogen doping synergistically modulates the electronic configuration of carbon, where fluorine reduces the Na+ adsorption energy barrier through strong electronegativity, while nitrogen introduces metastable adsorption sites. Guided by this insight, we developed fluorine and nitrogen co-doped porous hard carbon nanosheets (FN–HC) through a space-confined molten salt pyrolysis method, which function as both the anode and cathode in SIHCs. Mechanistic studies combining operando spectroscopy and molecular dynamics simulations reveal F/N-coordinated nanopockets enabling inorganic-rich (NaF) SEI layer with higher ionic diffusion coefficient than conventional organic-dominated interfaces. Moreover, the dual-active surface chemistry provides abundant adsorption sites, enhancing the anion (PF6-) adsorption/desorption capacitance. Consequently, the resulting AFN–HC//FN–HC SIHCs exhibit outstanding energy/power densities (154 Wh kg-1/8485 W kg-1) and long-term cycling stability (83.7 % capacity retention after 7000 cycles at 2 A g-1). This interface-kinetics co-regulation paradigm establishes a universal framework for designing multifunctional carbon architectures, bridging the gap between battery-type anodes and capacitor-type cathodes in hybrid energy storage systems. © 2025 Elsevier B.V.
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Energy Storage Materials
ISSN: 2405-8297
Year: 2025
Volume: 80
1 8 . 9 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 1
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