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Study of Higher Discharge Capacity, Phase Transition, and Relative Structural Stability in Li2FeSiO4 Cathode upon Lithium Extraction Using an Experimental and Theoretical Approach and Full Cell Prototype Study

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Energy Mater. 2019, 2, 9, 6584-6598
    Article

    Study of Higher Discharge Capacity, Phase Transition, and Relative Structural Stability in Li2FeSiO4 Cathode upon Lithium Extraction Using an Experimental and Theoretical Approach and Full Cell Prototype Study
    Click to copy article linkArticle link copied!

    • Shivani Singh
      Shivani Singh
      Electrochemical Energy Laboratory, Department of Energy Science and Engineering, Indian Institute of Technology, Bombay, Powai, Mumbai−400076, India
      More by Shivani Singh
    • Anish Raj K
      Anish Raj K
      Electrochemical Energy Laboratory, Department of Energy Science and Engineering, Indian Institute of Technology, Bombay, Powai, Mumbai−400076, India
      More by Anish Raj K
    • Manas Ranjan Panda
      Manas Ranjan Panda
      Electrochemical Energy Laboratory, Department of Energy Science and Engineering, Indian Institute of Technology, Bombay, Powai, Mumbai−400076, India
      IITB Monash Research Academy, Bombay, Mumbai−400076, India
      More by Manas Ranjan Panda
      Orcidhttp://orcid.org/0000-0003-4899-9522
    • Raja Sen
      Raja Sen
      Department of Physics, School of Natural Sciences, Shiv Nadar University, Gautam Budha Nagar, Greater Noida, Uttar Pradesh−201314, India
      More by Raja Sen
      Orcidhttp://orcid.org/0000-0002-9838-975X
    • Priya Johari*
      Priya Johari
      Department of Physics, School of Natural Sciences, Shiv Nadar University, Gautam Budha Nagar, Greater Noida, Uttar Pradesh−201314, India
      *Email: [email protected] (P.J.).
      More by Priya Johari
    • A. K. Sinha
      A. K. Sinha
      Indus Synchrotron Utilization Division, Raja Ramanna Centre for Advanced Technology, Indore−452013, India
      More by A. K. Sinha
    • Sher Singh Meena
      Sher Singh Meena
      Solid State Physics Division, Bhabha Atomic Research Centre, Mumbai−400085, India
      More by Sher Singh Meena
      Orcidhttp://orcid.org/0000-0003-4978-2528
    • Sagar Mitra*
      Sagar Mitra
      Electrochemical Energy Laboratory, Department of Energy Science and Engineering, Indian Institute of Technology, Bombay, Powai, Mumbai−400076, India
      *Email: [email protected] (S.M.).
      More by Sagar Mitra
      Orcidhttp://orcid.org/0000-0002-2604-5042
    Other Access OptionsSupporting Information (1)

    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2019, 2, 9, 6584–6598
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaem.9b01145
    Published August 8, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

    Abstract

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    We have revisited the study of the nanostructured lithium iron silicate-based cathode for a safe lithium-ion battery and to understand the reaction mechanism from the first cycle to the second cycle. Ex situ Mössbauer and X-ray absorption near edge structure spectroscopy (XANES) measurements have been carried out on electrodes charged at various voltages to investigate the electrochemical activity of the Fe3+/Fe4+ redox couple to confirm the existence of Fe4+ and its role in defining the structural and electrochemical properties. The first charge and discharge lead to a structural change, which results in a potential plateau shift after the first charge. To validate this understanding, ex situ synchrotron X-ray diffraction (SXRD) along with Rietveld refinement results and first-principles density functional theory-based analysis have been performed, which also support the change in the crystal structure of the material with cycling. The in situ electrochemical impedance spectroscopy demonstrates phase transformation in delithiated iron silicate as lithium concentration changes during the charging process, which has been correlated with change in the density of states calculated by density functional theory. Finally, a full-cell prototype has been demonstrated for the first time using a lithium iron silicate cathode as the cathode and graphite as the anode, and this full cell showed a capacity retention of 92% after 50 cycles at a 1 C rate.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsaem.9b01145.

    • SEM and TEM images, FTIR, simulated XRD, crystal structure, the density of states, and charge-discharge profile shown in Figures. Calculated distortion value in different tetrahedra, bader charge, bond length in Table (PDF)

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    Cited By

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    This article is cited by 22 publications.

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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2019, 2, 9, 6584–6598
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaem.9b01145
    Published August 8, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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