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

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. A synergistic effect is utilized for repairing defects of spent LiFePO4 (SLFP) at low temperature and constructing a multifunctional carbon layer with N/S doped on the surface of the regenerated LFP (RLFP). The electrochemical properties of the RLFP are improved due to the enhanced conductivity, structure protection, and the improved kinetics of Li+ transport.