In order to satisfy the escalating energy demands, it is inevitable to improve the energy density of current Li-ion batteries. As the development of high-capacity cathode materials is of paramount significance compared to anode materials, here we have designed for the first time a unique synergistic hybrid cathode material with enhanced specific capacity, incorporating cost-effective iron sulfide (FeS) nanoparticles in a sulfurized polyacrylonitrile (SPAN) nanofiber matrix through a rational in situ synthesis strategy. Previous reports on FeS cathodes are scarce and consist of an amorphous carbon matrix to accommodate the volume changes encountered during the cycling process. However, this inactive buffering matrix eventually increases the weight of the cell, reducing the overall energy density. By the rational design of this hybrid composite cathode, we ensure that the presence of covalently bonded sulfur in SPAN guarantees high sulfur utilization, while effectively buffering the volume changes in FeS. Meanwhile, FeS can compensate for the conductivity issues in the SPAN, thereby realizing a synergistically driven dual-active cathode material improving the overall energy density of the composite. Simultaneous in situ generation of FeS nanoparticles within the SPAN fiber matrix was carried out via electrospinning followed by a one-step heating procedure. The developed hybrid cathode material displays enhanced lithium-ion storage, retaining 688.6 mA h g(FeS@SPAN composite) –1 at the end of 500 cycles at 1 A g–1 even within a narrow voltage range of 1–3.0 V. A high discharge energy density > 900 W h kg(FeS@SPAN composite) –1, much higher than the theoretical energy density of the commercial LiCoO2 cathode, was also achieved, revealing the promising prospects of this hybrid cathode material for high energy density applications.

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A highly ordered mesoporous sulfurized polyacrylonitrile (MSPAN) composite has been synthesized via in situ polymerization of polyacrylonitrile (PAN) in an SBA-15 template followed by sulfurization. The synthesized composite possessed high sulfur utilization, high Coulombic efficiency, and excellent cycling stability as a cathode active material for high-rate lithium sulfur (Li−S) batteries. A highly ordered mesoporous structure was observed in the MSPAN composite from transmission electron microscopy. Excellent electrochemical and stable cycling performances of the MSPAN composite were obtained, especially at high C rates. The capacity retention of the MSPAN cell was 755 mAh g −1 after 200 cycles at 1 C and 610 mAh g −1 after 900 cycles at 2 C. Even at a higher rate of 5 C, the composite showed reasonable capacity retention. The superior performance of the MSPAN composite was attributed to its highly porous structure, which could effectively improve the wettability, accessibility, and absorption of electrolyte, facilitating rapid ion transfer in Li−S batteries. The electrochemical results demonstrate that the highly ordered mesoporous MSPAN composite is a promising cathode active material for advanced Li−S batteries.

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The study details the electrochemical characterization of NVP anodes and symmetric NVP cells in a DME electrolyte for the first time.