RESYNTHESIS AND ELECTROCHEMICAL PERFORMANCE OF NCM111 USING ULTRASOUND-ASSISTED LEACHATE FROM SPENT LITHIUM-ION BATTERY CATHODES

Honghao Yu; Junhui Ye; Nianping Li; Xin Li

doi:10.17222/mit.2025.1431

Honghao Yu School of Materials Science and Engineering, Shenyang Ligong University, Shenyang, Liaoning 110159, China
Junhui Ye School of Materials Science and Engineering, Shenyang Ligong University, Shenyang, Liaoning 110159, China
Nianping Li School of Materials Science and Engineering, Shenyang Ligong University, Shenyang, Liaoning 110159, China
Xin Li School of Materials Science and Engineering, Shenyang Ligong University, Shenyang, Liaoning 110159, China

DOI: https://doi.org/10.17222/mit.2025.1431

Keywords: spent lithium-ion batteries, ultrasound-assisted leachate, resynthesis, deep eutectic solvent, LiNi1/3Co1/3Mn1/3O2

Abstract

The widespread use of lithium-ion batteries (LIBs) led to a substantial accumulation of spent cathode materials, creating an urgent need for environmentally sustainable recycling methods that address both ecological concerns and the recovery of critical metals. A novel strategy integrating ultrasound-assisted deep eutectic solvent (DES) leaching and urea-assisted co-precipitation for the regeneration of high-performance LiNi₁/₃Co₁/₃Mn₁/₃O₂ (NCM111) cathodes from spent LiCoO₂ was developed. The results revealed that the transition metal-to-urea molar ratio critically governs the structural and electrochemical properties of regenerated materials. An NCM111 sample with an optimized transition metal-to-urea ratio of 1:2 had an ordered layered structure (I(003)/I(104) = 1.336), uniform spherical secondary particles (1–3 µm), and minimal cation mixing. These structural advantages translated into exceptional electrochemical performance, including an initial Coulombic efficiency of 84.84 %, 96.13 % capacity retention after 30 cycles, low charge-transfer resistance (37.26 Ω), and enhanced redox reversibility (ΔE_p = 0.21 V). Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) further confirmed the superior interfacial kinetics and reaction reversibility of the optimised sample.

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