Metastable Marcasite-FeS2 as a New Anode Material for Lithium Ion Batteries: CNFs-Improved Lithiation/Delithiation Reversibility and Li-Storage Properties

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Abstract
Marcasite (m-FeS2) exhibits higher electronic conductivity than that of pyrite (p-FeS2) because of its lower semiconducting gap (0.4 vs 0.7 eV). Meanwhile, as demonstrates stronger Fe–S bonds and less S–S interactions, the m-FeS2 seems to be a better choice for electrode materials compared to p-FeS2. However, the m-FeS2 has been seldom studied due to its sophisticated synthetic methods until now. Herein, a hierarchical m-FeS2 and carbon nanofibers composite (m-FeS2/CNFs) with grape-cluster structure was designed and successfully prepared by a straightforward hydrothermal method. When evaluated as an electrode material for lithium ion batteries, the m-FeS2/CNFs exhibited superior lithium storage properties with a high reversible capacity of 1399.5 mAh g–1 after 100 cycles at 100 mA g–1 and good rate capability of 782.2 mAh g–1 up to 10 A g–1. The Li-storage mechanism for the lithiation/delithiation processes of m-FeS2/CNFs was systematically investigated by ex situ powder X-ray diffraction patterns and scanning electron microscopy. Interestingly, the hierarchical m-FeS2 microspheres assembled by small FeS2 nanoparticles in the m-FeS2/CNFs composite converted into a mimosa with leaves open shape during Li+ insertion process and vice versa. Accordingly, a “CNFs accelerated decrystallization–recrystallization” mechanism was proposed to explain such morphology variations and the decent electrochemical performance of m-FeS2/CNFs.
Funding Information
  • National Natural Science Foundation of China (21274017, 21573036)
  • Research Center of Advanced Energy Materials, Northeast Normal University
  • Department of Education of Jilin Province (111099108)
  • Jilin Province (20150520027JH)

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