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Practical Implementation of Magnetite-Based Conversion-Type Negative Electrodes via Electrochemical Prelithiation.

Buse Bulut Kopuklu1, Ekin Esen2, Aurora Gomez-Martin3

  • 1Faculty of Engineering and Natural Sciences (FENS), Sabancı University, Üniversite Caddesi 27, 34956 Istanbul, Turkey.

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Electrochemical prelithiation significantly enhances the performance of magnetite-decorated partially reduced graphene oxide (Fe3O4@PrGO) negative electrodes in lithium-ion batteries. This process improves initial Coulombic efficiency and doubles capacity retention, paving the way for practical conversion electrode applications.

Keywords:
active lithium lossmagnetite (Fe3O4)partially reduced graphene oxideprelithiationsolid electrolyte interphase

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Conversion-type negative electrodes, such as magnetite-decorated partially reduced graphene oxide (Fe3O4@PrGO), offer high theoretical capacities for lithium-ion batteries.
  • Practical implementation of these electrodes in full cells is hindered by issues like active lithium loss and poor cycle life, primarily due to undesirable side reactions.
  • Electrochemical prelithiation is a potential strategy to mitigate these challenges by forming a stable solid electrolyte interphase (SEI) layer.

Purpose of the Study:

  • To investigate the impact of electrochemical prelithiation on the performance of Fe3O4@PrGO negative electrodes in a full-cell configuration with LiNi0.8Co0.15Al0.05O2 (NCA) positive electrodes.
  • To demonstrate the effectiveness of prelithiation in improving initial Coulombic efficiency (ICE) and long-term cycling stability.
  • To elucidate the mechanisms by which prelithiation enhances electrode passivation and reduces detrimental side reactions.

Main Methods:

  • Fabrication of Fe3O4@PrGO composite material for use as a negative electrode.
  • Assembly of full cells using Fe3O4@PrGO negative electrodes and NCA positive electrodes.
  • Electrochemical prelithiation of the Fe3O4@PrGO electrode to 35% of its specific delithiation capacity.
  • Galvanostatic cycling, electrochemical impedance spectroscopy (EIS), and surface analysis to evaluate cell performance and electrode behavior.

Main Results:

  • Electrochemical prelithiation improved the initial Coulombic efficiency (ICE) of the full cells from 70.8% to 91.2%.
  • Prelithiated Fe3O4@PrGO electrodes exhibited enhanced surface passivation, leading to reduced electrolyte reduction, lower polarization, and doubled capacity retention after 100 cycles.
  • Full cells with prelithiated negative electrodes showed a retained capacity of 60.4% after long-term cycling, which is three times higher than that of non-prelithiated cells.

Conclusions:

  • Electrochemical prelithiation is a highly effective strategy for mitigating active lithium losses and improving the cycle life of conversion-type Fe3O4@PrGO negative electrodes in full cells.
  • The improved performance is attributed to enhanced surface passivation, reduced electrolyte decomposition, and a stabilized SEI layer.
  • This study demonstrates that electrochemical prelithiation is a promising approach for advancing the practical application of conversion negative electrode materials in lithium-ion batteries.