Surface Spin-State Manipulation via a Strong Electronegative Ligand Field Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes

Authors: Jia, K., Ji, G., He, Y., Piao, Z., Zhang, M., Cao, Z., Li, C., Hou, K., Abdelkader, A.M., Liang, Z., Kumar, R.V., Ding, S., Zhou, G., Xi, K.

Journal: Angewandte Chemie International Edition

Publication Date: 01/01/2026

eISSN: 1521-3773

ISSN: 1433-7851

DOI: 10.1002/anie.2888520

Abstract:

The rapid growth of lithium-ion batteries has intensified the need for efficient recycling of spent LiNi0.5Co0.2Mn0.3O2 (NCM) cathodes. However, direct regeneration is hindered by the high-spin state of Ni2+ (S = 1) in degraded surface structures, which impedes Li+ intercalation and limits repair efficiency. Here, we introduce a strong electronegative ligand field to modulate the surface NiO6 coordination environment, enabling precise regulation of Ni spin state and electronic structure. This strategy alters the occupancy of Ni eg orbitals, converting high-spin Ni2+ (t2g6eg2, S = 1) to low-spin Ni3+ (t2g6eg1, S = 1/2) while downshifting the Ni d-band center. The resulting electronic reconfiguration weakens Ni-Li interactions, enabling efficient lithiation and regeneration of the degraded NCM black mass. The regenerated cathode, when assembled into pouch cells, exhibits Ah-level capacity with electrochemical performance comparable to commercial counterparts. This work establishes a direct correlation between Li+ transport kinetics and the Ni spin-state regulation, offering a new chemical paradigm for the direct regeneration of degraded cathodes.

Source: Scopus

Surface Spin-State Manipulation via a Strong Electronegative Ligand Field Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes.

Authors: Jia, K., Ji, G., He, Y., Piao, Z., Zhang, M., Cao, Z., Li, C., Hou, K., Abdelkader, A.M., Liang, Z., Kumar, R.V., Ding, S., Zhou, G., Xi, K.

Journal: Angew Chem Int Ed Engl

Publication Date: 26/05/2026

Pages: e2888520

eISSN: 1521-3773

DOI: 10.1002/anie.2888520

Abstract:

The rapid growth of lithium-ion batteries has intensified the need for efficient recycling of spent LiNi0.5Co0.2Mn0.3O2 (NCM) cathodes. However, direct regeneration is hindered by the high-spin state of Ni2+ (S = 1) in degraded surface structures, which impedes Li+ intercalation and limits repair efficiency. Here, we introduce a strong electronegative ligand field to modulate the surface NiO6 coordination environment, enabling precise regulation of Ni spin state and electronic structure. This strategy alters the occupancy of Ni eg orbitals, converting high-spin Ni2+ (t2 g 6eg 2, S = 1) to low-spin Ni3+ (t2 g 6eg 1, S = 1/2) while downshifting the Ni d-band center. The resulting electronic reconfiguration weakens Ni-Li interactions, enabling efficient lithiation and regeneration of the degraded NCM black mass. The regenerated cathode, when assembled into pouch cells, exhibits Ah-level capacity with electrochemical performance comparable to commercial counterparts. This work establishes a direct correlation between Li+ transport kinetics and the Ni spin-state regulation, offering a new chemical paradigm for the direct regeneration of degraded cathodes.

Source: PubMed

Surface Spin-State Manipulation via a Strong Electronegative Ligand Field Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes

Authors: Jia, K., Ji, G., He, Y., Piao, Z., Zhang, M., Cao, Z., Li, C., Hou, K., Abdelkader, A.M., Liang, Z., Kumar, R.V., Ding, S., Zhou, G., Xi, K.

Journal: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

Publication Date: 26/05/2026

eISSN: 1521-3773

ISSN: 1433-7851

DOI: 10.1002/anie.2888520

Source: Web of Science

Surface Spin-State Manipulation via a Strong Electronegative Ligand Field Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes.

Authors: Jia, K., Ji, G., He, Y., Piao, Z., Zhang, M., Cao, Z., Li, C., Hou, K., Abdelkader, A.M., Liang, Z., Kumar, R.V., Ding, S., Zhou, G., Xi, K.

Journal: Angewandte Chemie (International ed. in English)

Publication Date: 05/2026

Pages: e2888520

eISSN: 1521-3773

ISSN: 1433-7851

DOI: 10.1002/anie.2888520

Abstract:

The rapid growth of lithium-ion batteries has intensified the need for efficient recycling of spent LiNi0.5Co0.2Mn0.3O2 (NCM) cathodes. However, direct regeneration is hindered by the high-spin state of Ni2+ (S = 1) in degraded surface structures, which impedes Li+ intercalation and limits repair efficiency. Here, we introduce a strong electronegative ligand field to modulate the surface NiO6 coordination environment, enabling precise regulation of Ni spin state and electronic structure. This strategy alters the occupancy of Ni eg orbitals, converting high-spin Ni2+ (t2 g 6eg 2, S = 1) to low-spin Ni3+ (t2 g 6eg 1, S = 1/2) while downshifting the Ni d-band center. The resulting electronic reconfiguration weakens Ni-Li interactions, enabling efficient lithiation and regeneration of the degraded NCM black mass. The regenerated cathode, when assembled into pouch cells, exhibits Ah-level capacity with electrochemical performance comparable to commercial counterparts. This work establishes a direct correlation between Li+ transport kinetics and the Ni spin-state regulation, offering a new chemical paradigm for the direct regeneration of degraded cathodes.

Source: Europe PubMed Central