Transforming Retired LiFePO<sub>4</sub> Material toward High-Performance Cathodes for Sodium-Ion Batteries via Intermediate Phase-Guided Reconstruction.

Yang, Zhuoli; Wang, Peng; Xing, Chunxian; Chen, Jiaqi; Yang, Peng; Zhou, Jian; Chen, Long; Tao, Shuqiang et al. · ACS Nano · 2025

basic_science · Level V

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Abstract

Current recycling strategies for spent lithium iron phosphate (LiFePO<sub>4</sub>)-based batteries mainly concentrate on the extraction of the high-value lithium element via metallurgical processes, leaving the leached iron phosphate (FePO<sub>4</sub>) as trash. This poses serious environmental hazards and is a significant waste of materials. In this study, a two-step strategy is proposed to controllably convert leached LiFePO<sub>4</sub> material into a high-performance cathode material (Na<sub>3.12</sub>Fe<sub>2.44</sub>(P<sub>2</sub>O<sub>7</sub>)<sub>2</sub>) for sodium-ion batteries, which includes an elemental compensation step and a subsequent intermediate phase-guided structural transformation step. The product features well-dispersed nanoparticles with a uniform carbon coating. Furthermore, systematic <i>in situ</i> characterization extracts full details for the above conversion in terms of both reaction mechanisms and crystallization kinetics. The product, when used as cathode material in sodium-ion batteries, delivers exceptional capacity retention (97.5% after 800 cycles at 1 C) and excellent rate performance (a capacity of 45.7 mA h g<sup>-1</sup> at 30 C). This approach, which produces high-value emerging materials from waste materials, is economical, simple, and scalable, offering a sustainable solution for the efficient recycling of LiFePO<sub>4</sub>-based batteries.