Long‐Life Regenerated LiFePO<sub>4</sub> from Spent Cathode by Elevating the d‐Band Center of Fe
Kai Jia, Jun Ma, Junxiong Wang, Zheng Liang, Guanjun Ji, Zhihong Piao, Runhua Gao, Yanfei Zhu, Zhaofeng Zhuang, Guangmin Zhou, Hui–Ming Cheng
Abstract
Abstract A large amount of spent LiFePO 4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li + diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li + migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d‐band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen‐doped carbon. The FeO bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d‐band center. The Li + diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.