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<p>Developing binder-free electrodes with superior rate capability and cycling stability is critical for supercapacitors, yet remains challenging. Although NiCo<sub>2</sub>S<sub>4</sub> (NCS) nanoarrays exhibit high capacity and conductivity, their practical application is limited by poor rate performance and structural degradation. Herein, we synthesize Mn-doped NiCo<sub>2</sub>S<sub>4</sub> (Mn-NCS) hollow nanoneedle arrays directly on Ni foam via hydrothermal methods. Optimized Mn<sub>0.2</sub>-NCS achieves an exceptional specific capacitance of 8.92 F cm<sup>−2</sup> (1749 F g<sup>−1</sup>) at 1&#xa0;mA&#xa0;cm<sup>−2</sup> and retains 73.4% capacitance at 15&#xa0;mA&#xa0;cm<sup>−2</sup>, far exceeding undoped NCS (45.4%). The electrode also maintains 90.6% capacity retention after 5000 cycles at 15&#xa0;mA&#xa0;cm<sup>−2</sup>, demonstrating unparalleled stability. Experimental characterization reveals Mn doping reduces ion diffusion resistance (12.1 vs. 20.8 Ω s<sup>−1</sup> for NCS) and promotes surface-dominated charge storage (61.6% capacitive contribution at 1&#xa0;mV&#xa0;s<sup>−1</sup>). Density functional theory calculations confirm enhanced structural stability, increased electronic states near the Fermi level and significantly strengthened OH<sup>−</sup> adsorption energy. This work establishes Mn doping as an effective strategy to engineer high-performance ternary sulfide electrodes.</p>

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Boosting the rate capability and cycling stability of binder-free NiCo2S4 nanoarray electrodes via manganese doping

  • 期刊论文

  • 发表日期：

    2025年10月7日

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  • Lei Xiao,
  • Fan Tian,
  • Yanchao Zhang,
  • Fan Zhang,
  • Zhenglong Hu,
  • Shensong Wang,
  • Juan Xiong

摘要

Developing binder-free electrodes with superior rate capability and cycling stability is critical for supercapacitors, yet remains challenging. Although NiCo2S4 (NCS) nanoarrays exhibit high capacity and conductivity, their practical application is limited by poor rate performance and structural degradation. Herein, we synthesize Mn-doped NiCo2S4 (Mn-NCS) hollow nanoneedle arrays directly on Ni foam via hydrothermal methods. Optimized Mn0.2-NCS achieves an exceptional specific capacitance of 8.92 F cm−2 (1749 F g−1) at 1 mA cm−2 and retains 73.4% capacitance at 15 mA cm−2, far exceeding undoped NCS (45.4%). The electrode also maintains 90.6% capacity retention after 5000 cycles at 15 mA cm−2, demonstrating unparalleled stability. Experimental characterization reveals Mn doping reduces ion diffusion resistance (12.1 vs. 20.8 Ω s−1 for NCS) and promotes surface-dominated charge storage (61.6% capacitive contribution at 1 mV s−1). Density functional theory calculations confirm enhanced structural stability, increased electronic states near the Fermi level and significantly strengthened OH− adsorption energy. This work establishes Mn doping as an effective strategy to engineer high-performance ternary sulfide electrodes.