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

We report the performance of a conversion-type magnetite-decorated partially reduced graphene oxide (Fe₃O₄@PrGO) negative electrode material in full-cell configuration with LiNi_0.8Co_0.15Al_0.05O₂ (NCA) positive electrodes. To enable practical implementation of the conversion-type negative electrodes in full cells, the beneficial impact of electrochemical prelithiation on mitigating active lithium losses and improving cycle life is shown here for the first time in the literature. The initial Coulombic efficiency (ICE) of the full cells is improved from 70.8 to 91.2% by prelithiation of the negative electrode to 35% of its specific delithiation capacity. The prelithiation is shown to improve the surface passivation of the Fe₃O₄@PrGO electrodes, leading to less electrolyte reduction on their surface which is prominent from the significantly lowered accumulated Coulombic inefficiency values, lower polarization growth, and doubled capacity retention by the 100th cycle. The reduced surface reactions of the negative electrode by prelithiation also aids in reducing the extent of aging of the NCA positive electrode. Overall, the prelithiation leads to a longer cycle life, where a retained capacity of 60.4% was achieved for the prelithiated cells by the end of long-term cycling, which is 3 times higher than the capacity retention of the non-prelithiated cells. Results reported herein indicate for the first time that the electrochemical prelithiation of the Fe₃O₄@PrGO electrode is a promising approach for making conversion negative electrode materials more applicable in lithium-ion batteries.