文献类型：期刊文献

英文题名：Towards economically feasible recycling of spent LiFePO4 black mass: a thermodynamic-assisted targeted delithiation strategy

作者：Chen, Dongxian[1,2,3];Zhou, Shiyu[1,2,3];Wu, Siyu[1,2,3];Gu, Shuai[1,2,3];Yu, Jianguo[1,2,3]

机构：[1]East China Univ Sci & Technol, Natl Engn Res Ctr Integrated Utilizat Salt Lake, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Engn Res Ctr Salt Lake Resources Proc Engn, Minist Educ, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Joint Int Lab Potassium & Lithium Strateg Resource, Shanghai 200237, Peoples R China

年份：2026

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20261720583659);WOS:【SCI-EXPANDED(收录号:WOS:001746745800001)】；

基金：This work was supported by the National Natural Science Foundation of China (grant numbers 52304422 and 52554011), the Major Research Plan of the National Natural Science Foundation of China [grant number 92475207], and the Shanghai Rising-Star Program [grant number 24QA2702000] and the Technical Standards Project (grant number 25DZ2200600) of the Science and Technology Commission of Shanghai Municipality (STCSM).

语种：英文

外文关键词：Electronic Waste - Iron compounds - Lithium - Lithium compounds - Lithium-ion batteries - Phosphorus compounds - Reaction kinetics - Recycling - Thermodynamics

摘要：The recycling of spent LiFePO4 batteries is hindered by economic inefficiencies, primarily due to poor selectivity during lithium recovery. Here, we introduce a thermodynamic-assisted electrochemical delithiation strategy to achieve high-purity lithium extraction. By refining the thermodynamic models of the Li-Fe-P-H2O system, we delineate a precise operational window (pH 4.0-5.2 and an oxidation potential of 0.15-0.4 V) that favors Li+ removal while stabilizing the FePO4 framework, as verified by in situ electrochemical quartz crystal microbalance measurements. Crucially, we uncover that trace yet persistent iron dissolution originates from a proton-coupled reaction that forms an unstable HFePO4 intermediate, a previously overlooked mechanism that redefines the stability limits of the material in aqueous media. This study establishes a targeted, energy-efficient recycling pathway and provides fundamental insights into ion-exchange dynamics in olivine-type cathodes.