Targeted Defect Repair and Multi‐functional Interface Construction for the Direct Regeneration of Spent LiFePO₄ Cathodes

Abstract Due to the low economic benefits and environmental pollution of traditional recycling methods, the disposal of spent LiFePO₄ (SLFP) presents a significant challenge. The capacity fade of SLFP cathode is primarily caused by lithium loss and formation of a Fe (III) phase. Herein, a synergistic repair effect is proposed to achieve defect repair and multi‐functional interface construction for the direct regeneration of SLFP. Tannic acid (TA) forms a compact coating precursor for a carbon layer on SLFP with abundant functional groups and creates a mildly acidic environment to enhance the reducibility of thiourea (TU). Therefore, TU reduces Fe (III) to Fe (II) and repairs Li‐Fe anti‐site defects of SLFP, while at the same time acting as a source of N/S‐doping elements for the carbon layer at a lower temperature (140 °C). The multi‐functional carbon layer improves the properties of the regenerated LiFePO₄ (RLFP) due to the enhanced conductivity, structure maintenance and protection, and the improved kinetics of Li⁺ transport. Furthermore, the Fe─O and P─O bonds are strengthened, further enhancing the structural stability of the RLFP. Consequently, the RLFP demonstrates outstanding performance with a discharge capacity of 141.3 mAh g⁻¹ and capacity retention of 72% after 1000 cycles at 1 C.