Enhanced Prelithiation Performance of Li5FeO4 Cathode Additive and Optimized Solid Electrolyte Interface enabled by Mn Substitution

In the pursuit of enhancing the energy density of lithium-ion batteries, cathode prelithiation emerges as a pivotal approach, introducing additional irreversible active lithium ions to augment performance. Li5FeO4 (LFO) stands out as an excellent option, boasting an impressive theoretical specific capacity and the additional advantages of cost-effectiveness in raw materials and low preparation cost. However, the impact of extra lithium incorporations on compositional changes at the electrode-electrolyte interface as well as on cell stability has impeded further researches. Herein, a Mn doping strategy is proposed and predicted by first-principles calculations to synthesize partially Mn-substituted Li5.125Fe0.875Mn0.125O4 (LFMO). And the prelithiation with LFMO improved the interfacial composition of LiFePO4 (LFP) batteries compared to LFO, achieving a charging capacity of 213 mAh∙g-1 in the first cycle at 0.05C. The subsequent treatment demonstrated superior cycling stability, maintaining a discharge specific capacity as high as 155.3 mAh∙g-1 after 100 cycles at 0.2C, and exhibiting a higher capacity retention in the full cell. These discoveries could contribute to enhancing the regulation of battery interface during the utilization of LFO, potentially promoting the development of cathode lithium additives.