Recovering LiFePO_(4) extraction slag(LES)-the FePO_(4)-rich residue formed after Li leaching from spent LiFePO_(4)-has become pivotal to minimizing resource losses,mitigating environmental risks,and advancing circula...Recovering LiFePO_(4) extraction slag(LES)-the FePO_(4)-rich residue formed after Li leaching from spent LiFePO_(4)-has become pivotal to minimizing resource losses,mitigating environmental risks,and advancing circularity in lithium-ion battery value chains.However,integrative frameworks that link closed-loop routes(returning to battery precursors/cathodes)with non-closed-loop upcycling are still limited,constraining process optimization and scale-up.This review synthesizes current progress in LES recycling with emphasis on maximizing recovery efficiency and product value.In closed-loop pathways,hydrometallurgical purification removes impurities to yield battery-grade FePO_(4) as an LiFePO_(4) precursor,while direct relithiation(e.g.,solid-state sintering aided by Li sources and reductants)restores Li and reduces Fe^(3+)to Fe^(2+),thereby regenerating LiFePO_(4) cathodes from LES.In non-closed-loop pathways,compositionally guided upcycling converts LES into advanced materials(e.g.,high-performance electrodes,highcapacity adsorbents),thereby broadening the techno-economic value propositions.We also distill lessons from early industrial practice,identifying constraints arising from feedstock variability,energy-cost coupling(thermal/chemical utilities),and product-quality assurance(battery-grade specifications).Finally,we map research directions-including data-driven feed characterization and process control,defecthealing relithiation strategies and interfacial engineering,quality grading and market pathways,and multi-scenario deployment-to enhance the technical and economic sustainability of LES recycling and accelerate its contribution to a circular battery economy.展开更多
基金financially supported by the National Key Research and Development Program of China(Nos.2023YFC3904800)the National Outstanding Young Scientists Fund(No.52125002)+6 种基金the National Science Foundation of China(No.22476073 and U24A20194)the Key Project of Jiangxi Provincial Research and Development Program(Nos.20223BBG74006and 20243BBI91001)the Jiangsu Special Fund on Technology Innovation of Carbon Dioxide Peaking and Carbon Neutrality(No.BT2024011)the China Postdoctoral Science Foundation(Nos.2024M751282 and 2025T180353)the“Thousand Talents Program”of Jiangxi Province(S2021GDQN2161)the Key Project of Ganzhou City Research and Development Program(No.2023PGX17350)the Key Laboratory of Jiangxi Province for Functional Biology and Pollution Control in Red Soil Regions(No.2023SSY02051)。
文摘Recovering LiFePO_(4) extraction slag(LES)-the FePO_(4)-rich residue formed after Li leaching from spent LiFePO_(4)-has become pivotal to minimizing resource losses,mitigating environmental risks,and advancing circularity in lithium-ion battery value chains.However,integrative frameworks that link closed-loop routes(returning to battery precursors/cathodes)with non-closed-loop upcycling are still limited,constraining process optimization and scale-up.This review synthesizes current progress in LES recycling with emphasis on maximizing recovery efficiency and product value.In closed-loop pathways,hydrometallurgical purification removes impurities to yield battery-grade FePO_(4) as an LiFePO_(4) precursor,while direct relithiation(e.g.,solid-state sintering aided by Li sources and reductants)restores Li and reduces Fe^(3+)to Fe^(2+),thereby regenerating LiFePO_(4) cathodes from LES.In non-closed-loop pathways,compositionally guided upcycling converts LES into advanced materials(e.g.,high-performance electrodes,highcapacity adsorbents),thereby broadening the techno-economic value propositions.We also distill lessons from early industrial practice,identifying constraints arising from feedstock variability,energy-cost coupling(thermal/chemical utilities),and product-quality assurance(battery-grade specifications).Finally,we map research directions-including data-driven feed characterization and process control,defecthealing relithiation strategies and interfacial engineering,quality grading and market pathways,and multi-scenario deployment-to enhance the technical and economic sustainability of LES recycling and accelerate its contribution to a circular battery economy.