Hierarchically nanofibers embedded with NiMnS nanocrystals as anode for high-performance lithium-ion batteries: Experimental and theoretical studies

[Display omitted] •A series of NiMnS/carbon fibers (CFs) was made as anodes by regulating Ni/Mn ratio.•NiMnS/CFs delivered the final discharge capacities of 730 mA h g−1at 0.1A g−1.•After 250 cycle, NiMnS/CFs exhibited 99% of capacity retention at 1 A g−1.•DFT predicts fast charge–discharge rate with low diffusion energy barrier for Li+.•NiMnS/CFs-based full cell shows a specific energy 529 W h kg−1 and stable durability. Transition metal sulfides (TMSs) have been appraised as promising anode materials for lithium-ion batteries (LIBs), however, the average conductivity and drastic pulverization produced by specific volume variation during discharge–charge cycles limit their practical application. To resolve these critical issues, an in-situ fabrication approach has been utilized to develop binary TMS-embedded carbon nanofibers (CFs) by regulating the loading of metallic (cationic) components. Herein, a series of NiMnS/CFs-n composites was prepared by controlling Ni/Mn feeding ratios (n) via successive electrospinning, carbonization and sulfidation method. The inventive engineering procedure provides excellent durability (∼99 % compared to 2nd cycle) up to 250 cycles at 1 A g−1 and superb rate performance for NiMnS/CFs-2.0 anode. The final discharge capacities of NiMnS/CFs-2.0 are 730, 608, 562, 468, 370, and 306 mA h g−1 at 0.1, 0.3, 0.5, 1, 3, and 5 A g−1, respectively. Theoretical calculations enable us to understand the role of typical Ni/Mn feeding ratio on electronic properties and confirm that the hybrid NiMnS/CFs-2.0 surface provides enhanced material conductivity, improved Li adsorption energies for S-top sites, and fast discharge–charge rate with low diffusion energy barrier. Meanwhile, the full-cell containing NiMnS/CFs-2.0 anode outperforms the commercialized graphite anode with a high specific energy of ∼529 W h kg−1 and stable durability, which also successfully enlightens a light bulb. The present study will provide a scalable and simple method to fabricate the integrated composite of binary TMS/CFs by proper cationic regulation and offer useful guidelines for commercial applications of TMS-based anode.