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Single-phase synthesis, average, electronic, and local structure and cathode properties of pyroxene type LiFeSi2O6

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Abstract

Single-phase LiFeSi2O6 with pyroxene structure was firstly synthesized via a hydrothermal route under specific conditions with optimal water amount. Using both synchrotron X-ray and neutron diffraction techniques, crystal structure refinement with the C2/c space group resulted in well converged anisotropic displacement parameters. The electron density distributions were calculated by the maximum-entropy method (MEM) and showed the difference in the Si-O bond before and after charging. A carbon composite with LiFeSi2O6 exhibited strongly enhanced electrochemical properties as the cathode for Li-ion batteries due to the improved electronic conductivity. The X-ray absorption near edge structure (XANES) spectra revealed the redox of iron was not involved in the charge and discharge processes, while other mechanisms for charge and discharge were predicted to be related to Si or O. The local structure was refined by pair distribution function (PDF) analysis of the synchrotron X-ray and neutron total scatterings, which indicated Li-ion diffusion as a one-dimensional path.

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Acknowledgments

The authors thank Dr. K. Osaka for technical support with the synchrotron XRD experiments at BL19B2, SPring-8 (Proposal Nos. 2016A1509 and 2016B1859). The authors also thank Dr. T. Honma and Dr. H. Ofuchi for technical support with the XAFS experiments at BL14B2, SPring-8 (Proposal Nos. 2017A1573 and 2017B1590). Synchrotron X-ray total scattering experiments with the BL04B2 beamline at SPring-8 were performed under Program No. 2017A1290 and we thank Dr. K. Ohara for supporting these experiments. The authors are grateful to Profs. T. Ishigaki and A. Hoshikawa at Ibaraki University for assistance with the neutron diffraction measurements with iMATERIA (BL20; Proposal No. 2016BM0010) at the Materials and Life Science Experimental Faculty of J-PARC. We acknowledge Profs. T. Otomo and K. Ikeda at the High Energy Accelerator Research Organization (KEK) for their help on the neutron total scattering measurements with NOVA (BL21; Proposal No. 2018A0011) at J-PARC.

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Authors and Affiliations

  1. Faculty of Science & Technology, Tokyo University of Science, 2641 Yamazaki, Noda-shi, Chiba, 278-8510, Japan

    Naoya Ishida, Taketoshi Tajima, Naoto Kitamura & Yasushi Idemoto

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  1. Naoya Ishida
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  2. Taketoshi Tajima
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  3. Naoto Kitamura
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  4. Yasushi Idemoto
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Correspondence to Naoya Ishida.

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Ishida, N., Tajima, T., Kitamura, N. et al. Single-phase synthesis, average, electronic, and local structure and cathode properties of pyroxene type LiFeSi2O6. Ionics 27, 925–933 (2021). https://doi.org/10.1007/s11581-020-03876-z

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  • DOI: https://doi.org/10.1007/s11581-020-03876-z

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