Universal and Normalized Regeneration of Heterogeneous Spent LiFePO4 via Mechanochemical Delithiation and Flash Relithiation
Yaduo Song , Hao Zhang , Sanqi Guo , Cheng Lin , Junyi Lian , Xin Hu , Jinming Guo , Dinggen Li , Minglei Cao , Zhiqiang Wang , Jinyu Wen , Yunhui Huang , Jia Xie , Yonggang Yao
Energy & Environmental Materials ›› 2026, Vol. 9 ›› Issue (4) : e70225
The global surging demand for lithium iron phosphate batteries necessitates efficient recycling strategies to ensure environmental sustainability and resource conservation. While direct regeneration is considered sustainable, its widespread adoption is hindered by three critical challenges: 1) heterogeneous and unquantifiable lithium loss across waste streams, 2) abnormal particle growth during high-temperature restoration, and 3) limited economic returns arising from the low-value elements and complex process. Here, we report a universal and scalable “x → 0 → 1” normalization strategy. All spent LixFePO4 is first reset to Li-free olivine FePO4 (x → 0) via mechanochemical delithiation, eliminating batch-specific variability. Benefiting from the olivine FePO4 with pre-existing Li+ diffusion channels and nonequilibrium kinetics, subsequent ultrafast heating resynthesis (UHR) restores stoichiometric lithium iron phosphate (0 → 1) in just 35 s, effectively suppressing particle coarsening while cutting energy/time consumption by >99% compared to furnace sintering. This approach accommodates diverse degradation levels and their mixture, yielding regenerated lithium iron phosphate with consistent capacity, superior rate capability (84.3 mAh g−1 at 10 C) and cycling stability (89.1% retention after 1000 cycles at 10 C), outperforming fresh commercial lithium iron phosphate (73.3 mAh g−1, 66.6%). Beyond regeneration, flash upcycling to lithium manganese iron phosphate further enhances energy density to 549 Wh kg−1. Techno-economic analysis confirms strong profitability (lithium iron phosphate: 4.86 $ kg−1 cell, lithium manganese iron phosphate: 10.98 $ kg−1 cell), low energy demand (6.56 MJ kg−1 cell), and reduced emissions (2.95 kg CO2-eq kg−1 cell). Our strategy therefore establishes a general and robust platform for closed-loop cathode recycling and upcycling.
normalized regeneration / selective lithium recovery / spent LiFePO4 / sustainable recycling / ultrafast heating resynthesis
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2026 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.
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