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Updated: Jan 9, 2026

A Protocol for Safe Lithiation Reactions Using Organolithium Reagents
Published on: November 12, 2016
H+/OH- Switchable Coordination Chemistry Enables Sustainable and Selective Critical Metal Recovery from Spent Li-Ion
Qiang Zeng1,2, Xuezhen Feng1, Songhe Yang1
1State Key Laboratory of Soil Pollution Control and Safety, MEE Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.
Abstract:
Sustainable end-of-life management of lithium-ion batteries (LIBs) is essential for minimizing environmental impact and enhancing supply chain resilience. Here, we present a novel H+/OH- switchable reversible coordination chemistry mechanism that utilizes a cost-effective, recyclable K4Fe(CN)6 aqueous solution for highly efficient and selective recovery of critical metals from various spent LIB cathodes. Under H+-rich acidic conditions, the LiCoO2 (LCO) cathode demonstrates a high Li leaching efficiency of 96.57%, while cobalt selectively reacts with K4Fe(CN)6 to precipitate as K0.5H1.5CoFe(CN)6·H2O. Subsequent OH--rich base treatment facilitates the stepwise recovery of cobalt from K0.5H1.5CoFe(CN)6·H2O to form CoOOH, achieving a 95.18% recovery efficiency and K4Fe(CN)6 regeneration. In situ powder X-ray diffraction and time-dependent Raman spectroscopy reveal the dynamic crystal structural evolution and reversible coordination chemistry between Co─O bonding in LiCoO2/CoOOH and Co─N bonding in K0.5H1.5CoFe(CN)6·H2O, driven by the H+/OH- pair in the K4Fe(CN)6 solution. This strategy is applicable for recovering critical metals from a wide range of LIBs cathodes (e.g., NCMs, LFP), offering significant techno-economic and environmental benefits, and lays the foundation for sustainable critical metals recycling from urban minerals beyond spent LIBs.
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