Lithium‐ion batteries (LIBs) are in great demand for their impressive successes in serving people's daily life. Concomitantly, recycling the retired LIBs has also aroused the enthusiasm of widespread studies due to its great significance in the sustainable development of LIBs. Among the spent LIBs, LiFePO4 (LFP) is the main force because of its widespread use in electric vehicles and grids due to its stability and favorable price. However, considering the low cost of LFP manufacture as well as the abundance of Fe and P, traditional metallurgy processes are not economically feasible for recycling LFP because of high energy consumption and tedious steps. Here, this work proposes a green recycling method to directly regenerate the degraded LFP electrode via an in situ electrochemical process with a functionalized prelithiation separator. Compared with the existing recycling strategies for LFP batteries, the proposed method takes full advantage of the degraded cathode scraps without destroying the original structure, greatly reducing the cost of the remanufacture of the cathode electrodes simply via a prelithiation technique.

The complexity of chemical compounds in lithium‐ion batteries (LIBs) results in great difficulties in the extraction of multiple transition metals, which have similar physicochemical characteristics. Here, we propose a novel strategy for selective extraction of nickel, cobalt, and manganese from spent LiNixCoyMn1−x−yO2 (NCM) cathode through the regulation of coordination environment. Depending on adjusting the composition of ligand in transition metal complexes, a tandem leaching and separation system is designed and finally enables nickel, cobalt, and manganese to enrich in the form of NiO, Co3O4, and Mn3O4 with high recovery yields of 99.1 %, 95.1 %, and 95.3 %, respectively. We further confirm that the combination of different transition metals with well‐designed ligands is the key to good selectivity. Through our work, fine‐tuning the coordination environment of metal ions is proved to have great prospects in the battery recycling industry.

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The complexity of chemical compounds in lithium‐ion batteries (LIBs) results in great difficulties in the extraction of multiple transition metals, which have similar physicochemical characteristics. Here, we propose a novel strategy for selective extraction of nickel, cobalt, and manganese from spent LiNixCoyMn1−x−yO2 (NCM) cathode through the regulation of coordination environment. Depending on adjusting the composition of ligand in transition metal complexes, a tandem leaching and separation system is designed and finally enables nickel, cobalt, and manganese to enrich in the form of NiO, Co3O4, and Mn3O4 with high recovery yields of 99.1 %, 95.1 %, and 95.3 %, respectively. We further confirm that the combination of different transition metals with well‐designed ligands is the key to good selectivity. Through our work, fine‐tuning the coordination environment of metal ions is proved to have great prospects in the battery recycling industry.