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<p>Lithium-sulfurized polyacrylonitrile (Li-SPAN) batteries are an advanced class of Li–S energy storage systems that effectively mitigate the polysulfide shuttle effect. However, conventional SPAN cathodes experience low active material retention (&lt; 40&#xa0;wt%) and sluggish electrochemical kinetics, which limit their practical application. To address these challenges, this study introduces a CoS<sub>2</sub>/NiS<sub>2</sub>@SeSPAN composite nanofiber membrane as a high-performance Li-SPAN cathode. The cathode was synthesized through electrospinning Co/Ni salts with PAN, followed by hydrothermal deposition of Ni-ZIF-67 and SeS<sub><i>x</i></sub>-assisted thermal treatment to form a CoS<sub>2</sub>/NiS<sub>2</sub> heterostructure within the SeSPAN matrix. Experimental validation and density functional theory simulations confirmed that the cathode electrolyte interphase layer effectively encapsulated the active material, extending the solid-state reaction pathway. This hierarchical porous architecture enabled a high active material loading of 59&#xa0;wt%, which considerably exceeds that of conventional SPAN-based cathodes. The three-dimensional interconnected fiber network maximized the exposure of the CoS<sub>2</sub>/NiS<sub>2</sub> heterojunction, while the metal sulfides increased the conductivity to facilitate efficient electron and ion transport. The intrinsic electric field within the CoS<sub>2</sub>/NiS<sub>2</sub> heterostructure further enhanced polysulfide adsorption and catalytic conversion, accelerating the electrochemical kinetics. As a result, the CoS<sub>2</sub>/NiS<sub>2</sub>@SeSPAN cathode had an initial discharge capacity of 678&#xa0;mAh&#xa0;g<sup>−1</sup> at 0.2C, maintaining 634&#xa0;mAh&#xa0;g<sup>−1</sup> at 0.5C. Remarkably, the battery maintained 98.2% of its capacity after 800 cycles, highlighting its outstanding long-term cycling stability. The substantial potential of CoS<sub>2</sub>/NiS<sub>2</sub>@SeSPAN for high-performance Li-SPAN batteries and the critical role of heterostructure engineering in next-generation energy storage technologies are highlighted in this study.</p> Graphical abstract <p></p>

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Enhanced performance of lithium-sulfurized polyacrylonitrile batteries via multifunctional CoS2/NiS2 heterostructures and intrinsic electric fields

  • 期刊论文

  • 发表日期：

    2025年8月11日

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  • Hao Liu,
  • Hai-Hui Liu,
  • Qiang Xu,
  • Xiao-Dong Shao,
  • Xiao Zhang,
  • Shu-Liang Lv,
  • Zhi-Jia Zhang,
  • Chang Ma,
  • Yan-Mei Jin

摘要

Lithium-sulfurized polyacrylonitrile (Li-SPAN) batteries are an advanced class of Li–S energy storage systems that effectively mitigate the polysulfide shuttle effect. However, conventional SPAN cathodes experience low active material retention (< 40 wt%) and sluggish electrochemical kinetics, which limit their practical application. To address these challenges, this study introduces a CoS2/NiS2@SeSPAN composite nanofiber membrane as a high-performance Li-SPAN cathode. The cathode was synthesized through electrospinning Co/Ni salts with PAN, followed by hydrothermal deposition of Ni-ZIF-67 and SeSx-assisted thermal treatment to form a CoS2/NiS2 heterostructure within the SeSPAN matrix. Experimental validation and density functional theory simulations confirmed that the cathode electrolyte interphase layer effectively encapsulated the active material, extending the solid-state reaction pathway. This hierarchical porous architecture enabled a high active material loading of 59 wt%, which considerably exceeds that of conventional SPAN-based cathodes. The three-dimensional interconnected fiber network maximized the exposure of the CoS2/NiS2 heterojunction, while the metal sulfides increased the conductivity to facilitate efficient electron and ion transport. The intrinsic electric field within the CoS2/NiS2 heterostructure further enhanced polysulfide adsorption and catalytic conversion, accelerating the electrochemical kinetics. As a result, the CoS2/NiS2@SeSPAN cathode had an initial discharge capacity of 678 mAh g−1 at 0.2C, maintaining 634 mAh g−1 at 0.5C. Remarkably, the battery maintained 98.2% of its capacity after 800 cycles, highlighting its outstanding long-term cycling stability. The substantial potential of CoS2/NiS2@SeSPAN for high-performance Li-SPAN batteries and the critical role of heterostructure engineering in next-generation energy storage technologies are highlighted in this study.

Graphical abstract