The environmentally friendly and
low-cost recycling of spent LiFePO4 (LFP) cathode material
has become an urgent problem. Herein,
a green and effective one-step hydrothermal approach was proposed
for the direct regeneration of spent LFP. LFP will lose part of its
lithium and convert into FePO4 (FP) during long-term cycles.
Thus, a supplement of lost lithium is essential to regenerate spent
LFP, and this is thermodynamically feasible to achieve under hydrothermal
conditions. The hydrothermal conditions of temperature, Li+ concentration, and reductant dosage were investigated. It was found
that enhancement of hydrothermal conditions was beneficial to supplementing
lithium, correspondingly improving the electrochemical performance.
Under the hydrothermal conditions of 200 °C for 3 h, 12 g Lâ1 of Li+, L/S = 6 mL gâ1, and 1.0 mL of reductant (for every 5 g of spent LFP), the regenerated
LFP displayed excellent discharge capacities of 146.2 mAh gâ1 at 0.2 C, 141.9 mAh gâ1 at 1 C, and 128.2 mAh
gâ1 at 5 C. Additionally, the capacity retention
reached up to 98.6% after 200 cycles at 1 C. This regeneration method
has been demonstrated to be of good economic benefit and energy savings,
which will provide technological support for the sustainable development
of the LIBs industry.