Probing Hybrid LiFePO 4 /FePO 4 Phases in a Single Olive LiFePO 4 Particle and Their Recovering from Degraded Electric Vehicle Batteries.

The recycling of LiFePO 4 from degraded lithium-ion batteries (LIBs) from electric vehicles (EVs) has gained significant attention due to resource, environment, and cost considerations. Through neutron diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy, we revealed continuous lithium loss during battery cycling, resulting in a Li-deficient state (Li 1- x FePO 4 ) and phase separation within individual particles, where olive-shaped FePO 4 nanodomains (5-10 nm) were embedded in the LiFePO 4 matrix. The preservation of the olive-shaped skeleton during Li loss and phase change enabled materials recovery. By chemical compensation for the lithium loss, we successfully restored the hybrid LiFePO 4 /FePO 4 structure to pure LiFePO 4 , eliminating nanograin boundaries. The regenerated LiFePO 4 (R-LiFePO 4 ) exhibited a high crystallinity similar to the fresh counterpart. This study highlights the importance of topotactic chemical reactions in structural repair and offers insights into the potential of targeted Li compensation for energy-efficient recycling of battery electrode materials with polyanion-type skeletons.