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<p>Pyrite (FeS<sub>2</sub>) thin films have attracted significant attention as promising cathode materials for lithium-ion batteries due to their high theoretical capacity, natural abundance, and environmental benignity. However, due to sulfur volatility during film deposition, achieving stoichiometric FeS<sub>2</sub> remains challenging. In this study, we investigate the effects of post-deposition sulfurization treatment on the chemical composition, crystal structure, and electrochemical performance of FeS<sub>2</sub> thin films synthesized by RF magnetron sputtering. The as-deposited films exhibit notable sulfur deficiency, with an S: Fe atomic ratio of 0.27:1, while a 4-hour sulfurization process improves the ratio to 1.97:1, approaching ideal stoichiometry. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy confirm the formation of the pyrite phase, and X-ray diffraction (XRD) and field effect emission scanning electron microscopy (FESEM) reveal enhanced crystallinity and polycrystalline growth. Electrochemical analysis using cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) demonstrates that sulfurized films deliver superior initial and long-term (100-cycle) discharge specific capacities compared to as-deposited samples. The improved performance is attributed to optimized surface stoichiometry, increased reducibility, and the formation of stable intermediate phases. These findings underscore the critical role of sulfurization in tuning the structural and electrochemical properties of FeS<sub>2</sub> thin-film cathodes and present a viable strategy for enhancing the performance and stability of conversion-type cathodes in lithium-ion batteries.</p>

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Enhancing the cathodic performance of FeS2 in lithium-ion batteries via sulfurization treatment

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月27日

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  • Clifford Denize,
  • Makhes K. Behera,
  • Sangram K. Pradhan,
  • Messaoud Bahoura

摘要

Pyrite (FeS2) thin films have attracted significant attention as promising cathode materials for lithium-ion batteries due to their high theoretical capacity, natural abundance, and environmental benignity. However, due to sulfur volatility during film deposition, achieving stoichiometric FeS2 remains challenging. In this study, we investigate the effects of post-deposition sulfurization treatment on the chemical composition, crystal structure, and electrochemical performance of FeS2 thin films synthesized by RF magnetron sputtering. The as-deposited films exhibit notable sulfur deficiency, with an S: Fe atomic ratio of 0.27:1, while a 4-hour sulfurization process improves the ratio to 1.97:1, approaching ideal stoichiometry. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy confirm the formation of the pyrite phase, and X-ray diffraction (XRD) and field effect emission scanning electron microscopy (FESEM) reveal enhanced crystallinity and polycrystalline growth. Electrochemical analysis using cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) demonstrates that sulfurized films deliver superior initial and long-term (100-cycle) discharge specific capacities compared to as-deposited samples. The improved performance is attributed to optimized surface stoichiometry, increased reducibility, and the formation of stable intermediate phases. These findings underscore the critical role of sulfurization in tuning the structural and electrochemical properties of FeS2 thin-film cathodes and present a viable strategy for enhancing the performance and stability of conversion-type cathodes in lithium-ion batteries.