Abstract
Over the past few decades, rechargeable lithium-ion batteries have become popular for a variety of applications, such as electric vehicles, smart grids, and portable energy devices. However, due to their limited capacity, stability, and lifespan, they are not suitable for advanced transportation applications. To overcome these challenges, researchers have investigated the use of low-cost, high-energy-density, and safe positive electrode materials for secondary lithium batteries, including lithium iron sulfide. In this particular study, our focus is to investigate the effect of highly electronegative anion doping on the properties of lithium iron sulfide cathode through the solid-state method. Our approach involves using both in-situ and ex-situ observations to establish a correlation between the Redox behavior and structural properties of the prepared cathode materials. We have designed and characterized the material using various techniques, such as X-ray absorption spectroscopy (XAS) and synchrotron-based X-ray diffraction (XRD). Scanning electron microscope (SEM) measurement was conducted to study the morphology of the cathode material. Transmission electron microscopy (TEM) was employed to further study the microstructure of the cathode material at an atomic level. We analyzed the electron density distribution of the modified cathode material using XANES measurement and studied the structural properties through synchrotron-based XRD. Our study has revealed that oxygen-doping helps to improve material stability. As a result, the modified cathode (with optimal oxygen doping) exhibited a 50% capacity enhancement compared to pristine after 100 cycles. We also observed a shift to a higher voltage oxidation plateau of the oxygen-doped cathode material which is due to the influence of anion substitution on the electrochemistry and charge storage mechanisms. In summary, our detailed characterization and experimental results demonstrate the potential of oxygen-doped Li2FeS2 as a promising cathode material for advanced lithium-ion battery applications. The study's detailed characterization and experimental results will be presented, along with future perspectives.
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