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<p>The present work focuses on resolving a critical interfacial issue in solid-state energy storage devices using a synergistic interface–bulk engineering strategy that achieves high performance parameters in Na<sup>+</sup>-ion supercapacitors based on a solid polymer electrolyte. Through controlled N, <i>N</i>-dimethylformamide (DMF) addition (~ 3–5&#xa0;μl&#xa0;cm<sup>−2</sup>), a gradient gel–polymer interface is created that reduces interfacial resistance by ~ 82% (from 140 to ~ 25&#xa0;Ω), efficiently increasing the electrode–electrolyte contact area. Combined with the incorporation of KI, the first successful addition of redox additives in a solid polymer electrolyte, our approach achieves a remarkably high specific capacitance of ~ 590&#xa0;F&#xa0;g<sup>−1</sup> through I<sup>−</sup>/I<sub>3</sub><sup>−</sup> redox chemistry. The practical applicability is demonstrated by powering an 8&#xa0;V light-emitting diode (LED) for &gt; 50&#xa0;min. Investigations reveal that DMF creates a ~ 20–30&#xa0;μm transitional zone with enhanced chain mobility without compromising bulk mechanical properties. Meanwhile, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) confirm that the modification does not lead to unwanted chemical reactions. The device exhibits excellent electrochemical stability, with ~ 76 and 50% capacitance retention after 2000 and 10000 galvanostatic charge–discharge cycles, respectively, and maintains a high coulombic efficiency of ≥ 99% at 1&#xa0;V/1&#xa0;mA. The investigation reveals that redox-active species can operate effectively even in a restricted liquid-free polymer matrix, paving the way for high performance, commercially viable solid-state energy storage.</p> Graphical Abstract <p></p>

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Interface modulation combined with redox additive strategies for improving solid-state Na+ ion supercapacitor performance

  • 期刊论文

  • 发表日期：

    2025年11月20日

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  • Neha,
  • Hardeep,
  • Bhargab Sharma,
  • Kamaldeep Bisht,
  • Anshuman Dalvi

摘要

The present work focuses on resolving a critical interfacial issue in solid-state energy storage devices using a synergistic interface–bulk engineering strategy that achieves high performance parameters in Na+-ion supercapacitors based on a solid polymer electrolyte. Through controlled N, N-dimethylformamide (DMF) addition (~ 3–5 μl cm−2), a gradient gel–polymer interface is created that reduces interfacial resistance by ~ 82% (from 140 to ~ 25 Ω), efficiently increasing the electrode–electrolyte contact area. Combined with the incorporation of KI, the first successful addition of redox additives in a solid polymer electrolyte, our approach achieves a remarkably high specific capacitance of ~ 590 F g−1 through I−/I3− redox chemistry. The practical applicability is demonstrated by powering an 8 V light-emitting diode (LED) for > 50 min. Investigations reveal that DMF creates a ~ 20–30 μm transitional zone with enhanced chain mobility without compromising bulk mechanical properties. Meanwhile, X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) confirm that the modification does not lead to unwanted chemical reactions. The device exhibits excellent electrochemical stability, with ~ 76 and 50% capacitance retention after 2000 and 10000 galvanostatic charge–discharge cycles, respectively, and maintains a high coulombic efficiency of ≥ 99% at 1 V/1 mA. The investigation reveals that redox-active species can operate effectively even in a restricted liquid-free polymer matrix, paving the way for high performance, commercially viable solid-state energy storage.

Graphical Abstract