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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Precise and controlled carbothermal reduction for selective lithium extraction from spent cathodes via double-enhancement process

Xue Bai,Yanzhi Sun,Jiahong Xie,Rui He,Lihui Zhang,Junqing Pan

Carbothermal reduction is considered to be an efficient and cost-effective method for the recovery of cathodes in spent lithium-ion batteries (S-LIBs). However, the conventional direct mixed roasting with high reaction temperature, slow solid phase reaction kinetics and uncontrollable reduction process greatly hinders the lithium recovery efficiency and carbon emission reduction. Here, we propose a dual super-liquid film reactors (SLFR) enhancement strategy to achieve nanoscale mixing of spent anode and cathode materials to improve the kinetics of the roasting and water leaching processes. This strategy reduces the reaction temperature and time to 550°C and 1 h, improves the mass transfer efficiency of the solid phase reaction and aqueous leaching, precisely reduces LCO to CoO instead of Co metal, increases the lithium leaching rate from 85.6 % to 98.6 %, shortens the leaching time from 60 min to 40 s, and reduces the carbon dosage from 5 % to the theoretical value of 3 %, achieving zero carbon emission from the reduction process. This work provides a new general strategy for efficient, clean and precise carbothermal reduction of spent cathode materials for selective lithium extraction, and demonstrates the scalability in industrial applications.

CAS / MDL: 616-38-6 872-50-4
研究领域: 材料科学 · 环境工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Study on deep synergistic leaching mechanism of spent lithium iron phosphate under the H2SO4-H2O2 system and precise chemical precipitation recovery strategy of lithium carbonate

Jun Cong,Shao-hua Luo,Qi Sun,Xin Liu,Yi-Kai Wang,Sheng-xue Yan,Peng-wei Li

Efficient leaching and recovery of LiFePO 4 (LFP) in spent lithium-ion batteries (LIBs) is a key step to realize the recycling of lithium resources. Herein, H 2 SO 4 -H 2 O 2 is selected as the leaching agent to achieve selective leaching of lithium from spent LFP cathode materials, and the response surface method (RSM) serves to define the optimal leaching process. The experimental findings signify that when the concentration of H 2 SO 4 is 0.315 mol·L -1 , H 2 O 2 /Li molar ratio of 2.13, H 2 SO 4 /Li molar ratio of 0.62 (solid–liquid ratio of 96.87 g·L -1 ), leaching temperature of 62 °C and leaching time of 90 min, the leaching rate of Li + can reach as high as 95.23 %. Thermodynamic analysis, infrared spectroscopy and Mössbauer spectrum are used to clarify the reaction mechanism, that is, Fe 2+ in LiFePO 4 is oxidized to Fe 3+ by H 2 O 2 in situ to form FePO 4 , and Li + is released into the solution. Moreover, chemical precipitation method is used to efficiently recover the lithium resources in the form of lithium carbonate. By applying Box-Behnken design (BBD) and RSM to optimize the recovery technology to reach the global optimal solution to achieve the highest recovery rate of Li + in spent LFP. The experimental results show that under the optimal conditions of a Na 2 CO 3 /Li molar ratio of 0.6, a reaction temperature of 90 °C, and a C (Li + ) of 20.28 g·L -1 , the precipitation rate of Li + reaches 89.22 %. Moreover, the physical properties of the recovered Li 2 CO 3 are analyzed, and the content of Li 2 CO 3 in the recovered product is as high as 99.62 %. Additionally, the economic analysis and environmental impact analysis of the whole process of hydrometallurgical recovery of cathode materials are carried out by EverBatt 2023 model, which confirmed that hydrometallurgy is the extremely satisfactory method for recovering spent LFP cathode materials.

研究领域: 环境科学 · 材料科学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Selective Lithium Leaching from Spent Lithium-Ion Batteries via a Combination of Reduction Roasting and Mechanochemical Activation

Yu Zhang,Jiangmin Guo,Meng Yu,Xingrui Li,Shaojun Liu,Hao Song,Weihong Wu,Chenghang Zheng,Xiang Gao

The pretreatment of cathode material from spent lithium-ion batteries is employed for the purpose of selective lithium leaching, which combines reduction roasting with mechanochemical activation without any additives. Under a nitrogen atmosphere (600 °C, 240 min), lithium in the cathode material changes into lithium salts and other metals transform into low-valence/elemental states via intricate reactions between LiMnxCoyNizO2 and inherent carbon. Then, the transition metals at low-valence and elemental states exhibit relatively slow leaching rates in a short time period, while lithium can efficiently migrate into solution. To further optimize this process, mechanochemical activation via ball milling (10 Hz, 30 min) is employed, decreasing the particle size and inducing a transition from crystal to an amorphous phase, facilitating the efficiency of lithium leaching. Under the low-temperature and short-duration leaching conditions (35 °C, 5 min, 2 mol/L H2SO4, 100 g/L), nearly 91.6% lithium is leached out, and the selectivity reaches 92.2%. The lithium solution is further purified by the extractant Versatic 10, and high-purity Li2CO3 is precipitated by adding Na2CO3. This method is also applied to selectively leach lithium from LiCoO2 and LiNiO2 cathodes, achieving remarkable leaching efficiencies of 95.8 and 100%, respectively.

CAS / MDL: 34819-78-8
研究领域: 材料科学 · 环境工程 · 化学工程 · 可持续能源
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CHEMPHYSCHEM · 2025 · IF 2.2

Tuning Li Leaching from Solid Electrolytes LATP in All-Solid-State Lithium-Ion Batteries by Ternary Component for Green and Efficient Recovery

Yu Chen,Zhenghui Liu,Zheng Li,Yanlong Wang,Qi Liu,Minghui Feng

Achieving high metal leaching efficiency via regulation strategy is essential for minimizing raw material waste and reducing waste generation in hydrometallurgy. However, conventional approaches of tuning temperature and time frequently result in increased equipment corrosion and increased industrial costs. Therefore, recycling waste solid-state battery relies on the development of new tuning strategies. Here, a new strategy is developed to tune the leaching efficiency of metals by amino acid-based low-melting mixture solvents from lithium aluminum titanium phosphate Li 1.3 Al 0.3 Ti 1.7 P 3 O 12 (LATP) in all-solid-state lithium-ion batteries. This novel strategy demonstrates a more pronounced metal leaching efficiency, resulting in an increase in the highest Li leaching efficiency from 48.0% to 78.2%. In comparison, tunability by solvent types, temperature, and time on Li efficiency is less efficient, with Li efficiency only varying from 44.9% to 52.3%, 37.7% to 51.0%, and 36.8% to 56.3%, respectively. Graphical A new and sustainable strategy is developed to tune the recycling of solid electrolyte LATP by adjusting ternary components in the biodegradable and biocompatible amino acid-based low-melting mixture solvents, achieving a significant increase in Li leaching efficiency from 48.0% to 78.2%, indicating a 1.6-fold enhancement.

研究领域: 材料科学 · 电化学 · 能源化学 · 环境工程 · 冶金工程 · 可持续技术
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