Electrospun FeS₂@Carbon Fiber Electrode as a High Energy Density Cathode for Rechargeable Lithium Batteries

Abstract

In this study, an FeS2@carbon fiber electrode is developed with FeS2 nanoparticles either embedded in or attached to carbon fibers by using an electrospinning method. By applying this binder-free, metal-current-collector-free FeS2@carbon fiber electrode, both the redox reaction and capacity decay mechanisms for the Li-FeS2 system are revealed by changing the electrolyte (conventional carbonate electrolyte and a "solvent-in-salt"-type Li-S battery electrolyte) and working voltage ranges (1.0-3.0 V and 1.5-3.0 V vs Li/Li(+)). The FeS2@carbon fiber electrode shows stable cycling performance in both the conventional carbonate electrolyte and the solvent-in-salt-type Li-S battery electrolyte in the voltage range of 1.5-3.0 V. Electrochemical tests in the solvent-in-salt-type Li-S battery electrolyte indicate that the Li-FeS2 system becomes a hybrid of the Li-S cell and Li-iron sulfide cell after the initial cycle. Based on the understanding on the capacity decay mechanisms, the cycling stability of the Li-FeS2 system in the voltage range of 1.0-3.0 V is then significantly enhanced by coating the FeS2@carbon fiber electrode with a thin layer of Al2O3. The Al2O3-coated electrode demonstrates excellent cycling performance with high discharge energy densities at both the material level (∼1300 Wh/kg-FeS2) and the electrode level (∼1000 Wh/kg-FeS2 electrode).