Citation: Xiaohui Zhao, Haigang Dong, Zitong Fei, Qi Meng, Peng Dong. Single-crystallization regeneration of spent cathode materials via sub-molten state thermodynamic regulation and fast ionic conductor interface construction[J]. Chinese Chemical Letters, ;2026, 37(12): 111565. doi: 10.1016/j.cclet.2025.111565 shu

Single-crystallization regeneration of spent cathode materials via sub-molten state thermodynamic regulation and fast ionic conductor interface construction

Xiaohui Zhao ^{a, d} ,
Haigang Dong ^b ,
Zitong Fei ^{c, *,} ,
Qi Meng ^{a, *,} ,
Peng Dong ^{a, *,}

a.
National and Local Joint Engineering Research Center for Lithium-ion Batteries and Materials Preparation Technology, Key Laboratory of Advanced Battery Materials of Yunnan Province, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China
b.
Sino-Platinum Metals Co., Ltd., Kunming 650000, China
c.
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China
d.
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua 321004, China

zitongfei@sz.tsinghua.edu.cn

mengqi315117@126.com

dongpeng@kust.edu.cn

Received Date: 21 May 2025
Revised Date: 8 July 2025
Accepted Date: 8 July 2025
Available Online: 18 July 2025

Figures(5)

The development of green and scientific recycling of spent lithium-ion batteries is closely intertwined with the sustained advancement of the new energy industry chain. However, direct regeneration has emerged as a superior alternative owing to its streamlined processes and high added-value advantages. In response to the pronounced grain boundary effects, poor structural stability, and severe interfacial side reactions in regenerated polycrystalline particles, this work proposes a synergistic strategy of thermodynamic regulation in sub-molten state and in situ self-formed modification with fast ionic conductor Li₃N phases for single-crystallization regeneration of spent LiNi_0.8Co_xMn_0.2-xO₂ materials. Based on thermodynamic regulation, the decomposition product NH₃ reacts with a lithium compensation agent, forming the fast ionic conductor Li₃N interface on the surface of regenerated single-crystal particles. Through the regulation of urea's thermodynamic behavior, urea penetrates along grain boundaries in the sub-molten state, thereby weakening the grain boundary bonding strength and inducing directional fracture. This process enables the fragmentation of spent polycrystalline materials into submicron-sized particles, ultimately achieving single-crystallization regeneration. This strategy has effectively restored and optimized the crystal structure of ternary materials, recovered their electrochemical performance, and enhanced the conductivity of regenerated materials while suppressing transition metal dissolution. Electrochemical tests demonstrate that the regenerated material delivers an initial capacity of 194.42 mAh/g and retains a discharge specific capacity of 158.9 mAh/g after 200 cycles. This effective strategy provides valuable insights into the single-crystallization regeneration of spent NCM cathodes from lithium-ion batteries
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