A study on the effects of different crushing methods on the surface properties of high-nickel electrode materials and related behavior in lithium recovery--颗粒学报PARTICUOLOGY

A study on the effects of different crushing methods on the surface properties of high-nickel electrode materials and related behavior in lithium recovery

Wenzhe Wang^a, Bu Chu^a, Xueying He^a, Shengmao Lin^a, Weining Xie^{a b *}, Linhan Ge ^c, Fengbin Zhang^d, Qisen Xue^e, Tao Zhang^e *

a School of Chemical Engineering, China University of Mining and Technology, Xuzhou, 221116, China
b Advanced Analysis & Computation, Center, China University of Mining and Technology, Xuzhou, 221116, China
c Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China
d Key Laboratory of Xinjiang Coal Resources Green Mining, Ministry of Education, Xinjiang Institute of Engineering, Urumqi, 830023, China
e Beichen Advanced Recycling Technology (Qingdao) Co., Ltd, Qingdao, 266041, China

10.1016/j.partic.2026.07.014

Volume 117, October 2026, Pages 262-274

E-mail: Received 14 May 2026, Revised 9 July 2026, Accepted 24 July 2026, Available online 25 July 2026, Version of Record 6 August 2026.

Highlights

• Charged-state crushing and post-discharge crushing exert different effects on the material structure and binder content.

• Organic components exhibit similar thermal mass-loss behavior after charged-state crushing and post-discharge crushing.

• Two pretreatment routes promote different lithium dissociation mechanisms in materials.

• Aluminum impurities in the black mass obtained through two pretreatment routes significantly affect material leaching.

Abstract

This study compared the effects of charged-state crushing and post-discharge crushing on the surface chemistry, thermal-reduction behavior, and water-leaching characteristics of spent nickel-rich electrode materials. Charged-state crushing disrupted the layered structure, reduced the surface coverage of binder residues, decreased the content of PVDF-related functional groups from 39% to 26%, and lowered the surface Ni3+ fraction from 70% to 56%. After thermal reduction at 500 °C for 1 h, the original layered phases of both samples were substantially destroyed, and lithium leaching efficiencies reached 71% and 75%, respectively. At lower temperatures, the post-discharge-crushed sample exhibited higher lithium extraction efficiency; the maximum difference, 12.57%, occurred at 550 °C, mainly due to Li+ redistribution into the cathode lattice during discharge. By contrast, lithium release from the charged-state-crushed sample relied more strongly on graphite-assisted carbothermic reduction and was limited by residual lithium in graphite/interfacial deposits and the formation of water-insoluble LiAlO2. At 700 °C, most NiO and CoO were reduced to metallic Ni and Co, and lithium leaching efficiency exceeded 90%. These results demonstrate that pretreatment routes affect efficient lithium recovery from spent nickel-rich lithium-ion batteries by regulating PVDF decomposition, Ni valence-state evolution, LiAlO2 formation, and lithium-release pathways.

Graphical abstract

Keywords

Spent nickel-rich electrode materials; Charged-state crushing; Post-discharge crushing; Lithium leaching; LiAlO₂

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