Bidirectional Lattice Anchoring Enhances Composition Reconfiguration of Spent Lithium-Ion Cathodes

TY - JOUR

T1 - Bidirectional Lattice Anchoring Enhances Composition Reconfiguration of Spent Lithium-Ion Cathodes

AU - Zhu, Ahui

AU - Fan, Ersha

AU - Zhang, Xiaodong

AU - Chen, Renjie

AU - Li, Li

N1 - Publisher Copyright: © 2026 Wiley-VCH GmbH.

PY - 2026/5/27

Y1 - 2026/5/27

N2 - High-value recycling of retired lithium-ion battery materials is pivotal for the circular economy. The nickel-rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi0.54Co0.16Mn0.3O2 (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre-anchoring Al species on both SNCM and Ni(OH)2 surfaces. This method reduces the energy barrier for lithiation in the surface-disordered structures of SNCM and suppresses the structural degradation of nickel-rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g−1 at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid-state regeneration and establishes a pathway toward the high-value recycling of degraded lithium-ion batteries, demonstrating great potential for practical application.

AB - High-value recycling of retired lithium-ion battery materials is pivotal for the circular economy. The nickel-rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi0.54Co0.16Mn0.3O2 (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre-anchoring Al species on both SNCM and Ni(OH)2 surfaces. This method reduces the energy barrier for lithiation in the surface-disordered structures of SNCM and suppresses the structural degradation of nickel-rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g−1 at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid-state regeneration and establishes a pathway toward the high-value recycling of degraded lithium-ion batteries, demonstrating great potential for practical application.

KW - bidirectional anchoring

KW - heterogeneous reaction

KW - nickel-enrichment

KW - stable layered structure

UR - https://www.scopus.com/pages/publications/105033845806

U2 - 10.1002/aenm.70869

DO - 10.1002/aenm.70869

M3 - Article

AN - SCOPUS:105033845806

SN - 1614-6832

VL - 16

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 20

M1 - e70869

ER -