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author:

Pan, D. (Pan, D..) [1] | Liu, Y. (Liu, Y..) [2] | Muhammad, M.A. (Muhammad, M.A..) [3] | Xu, L. (Xu, L..) [4] | Liang, P. (Liang, P..) [5] | Yang, K.R. (Yang, K.R..) [6] | Zhan, H. (Zhan, H..) [7] | Hu, X. (Hu, X..) [8] | Wen, Z. (Wen, Z..) [9]

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Scopus

Abstract:

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.

Keyword:

Fluorine/nitrogen dual-doped Janus Machine learning Porous hard carbon nanosheets Sodium-ion hybrid capacitors

Community:

  • [ 1 ] [Pan D.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 2 ] [Liu Y.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 3 ] [Muhammad M.A.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 4 ] [Xu L.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 5 ] [Liang P.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 6 ] [Yang K.R.]Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071, China
  • [ 7 ] [Zhan H.]College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 8 ] [Hu X.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China
  • [ 9 ] [Wen Z.]State Key Laboratory of Structural Chemistry, and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fujian, Fuzhou, 350002, China

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Source :

Energy Storage Materials

ISSN: 2405-8297

Year: 2025

Volume: 80

1 8 . 9 0 0

JCR@2023

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 1

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