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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

A green recyclable process for selective recovery of Li and Fe from spent lithium iron phosphate batteries by synergistic effect of deep eutectic solvent and oxygen

Yaozhi Zhang,Bingru Wang,Fang Wang,Yasen Dai,Shuhang Ren,Yucui Hou,Weize Wu

This work designs a new method for recovering spent LiFePO 4 cathode materials, aiming to address issues with traditional hydrometallurgy processes such as complex operations, low lithium recovery rates, and high wastewater discharge. The method involves using a deep eutectic solvent (DES) composed of chloroacetic acid and ethanol, and oxygen as an oxidant, for the cooperative leaching of LiFePO 4 powders. Based on the acidic nature of the DES and the oxidizing properties of oxygen, LiFePO 4 was undergone an in-situ transformation into solid FePO 4 , while 100% of lithium was dissolved in the DES with high selectivity. The FePO 4 product can be recovered by filtration, and the addition of oxalic acid to the filtrate allows for lithium recovery. Importantly, the structure of the DES remained unchanged after use, allowing for three recycling cycles without a significant decrease in LiFePO 4 recovery efficiency. This process is environmentally friendly, with no generation of acidic or alkaline wastewater, and boasts high metal recovery rates, showcasing its huge potential for application.

CAS / MDL: 144-62-7 15365-14-7
研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL RESEARCH · 2023 · IF 8.3

A simple green method for in-situ selective extraction of Li from spent LiFePO4 batteries by synergistic effect of deep-eutectic solvent and ozone

Shujie Tang,Ziyue Yang,Mei Zhang,Min Guo

Efficient and clean extraction lithium (Li) from spent LiFePO 4 batteries (LIBs) still remains a challenge. In this paper, a green deep eutectic solvent (DES) based on ethylene glycol (EG) and choline chloride (CC), combined with ozone (O 3 ) from air source, realized highly selective leaching Li from LiFePO 4 in situ for the first time. The influence of experimental parameters on Li and Fe leaching efficiencies ( η Li , η Fe ) were studied by orthogonal and single-factor tests, and η Li  ≥ 92.2% while η Fe  ≤ 1.6% were obtained under the optimal conditions (6 h, 20 g/L, 8EG:1CC, 40 °C). The impurity Fe in the filtrate was completely precipitated as amorphous FePO 4 ·3H 2 O after heating (150 °C, 0.5 h), achieving a pure Li-solution. The leaching mechanism elucidated that the synergistic effect (acidification, replacement and oxidation reaction) between the DES and O 3 determined the phase transition of Li and Fe, promoting the efficient selective extraction of Li and in-situ separation of Fe (FePO 4 ). The average η Li and η Fe were separately 85.4% and 2.0% after ten cycles of the 8EG:1CC, indicative of its’ excellent reusability. Meanwhile, LiCl was recovered from the filtrate. This process avoided the use of strong acid/alkali and discharge of waste water, providing fresh perspectives on the green recovery of spent LiFePO 4 batteries.

CAS / MDL: 67-48-1 15365-14-7
研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 39 ·51673-51686 · IF 0

Effective peroxymonosulfate activation by lithium cobaltite recovered from spent lithium-ion batteries for enhanced carbamazepine degradation in a wide pH range

Wang Xi,Hou Fali,Zhai Jinli,Yan Jiali,Gong Chao,Li Yinghao,Zhu Wenjie,Luo Yongming,Yang Daoli,Gao Xiaoya

Considering the high cost and complicated recycling process of spent lithium-ion batteries (SLIBs), transforming SLIBs into environment functional materials may be a wise approach. Herein, lithium cobaltite (LCO) cathode powders recovered from SLIBs were used to activate peroxymonosulfate (PMS) for removing carbamazepine (CBZ). The recovered LCO enables a 98.2% removal efficiency of CBZ (2.5 mg/L) within 10 min, which was effective at a broader pH range (pH = 5.0–11.0). The influence of key factors (initial pH, PMS, and catalyst dosage) and coexisting substances (SO 4 2− , H 2 PO 4 − , NO 3 − , Cl − , HCO 3 − , and HA) on CBZ degradation were examined in detail. The primary radical species during the degradation of CBZ were proved to be 1 O 2 , SO 4 − , and . OH that generated from PMS activation initiated by the valence change of Co in recovered LCO. The recovered LCO displayed excellent reusability with about 80.0% removal of CBZ after six cycles. Homogeneous activation of PMS mainly contributed to CBZ degradation in the first run, but the recovered LCO catalyst dominated the heterogeneous activation of PMS for the degradation of CBZ in the second to sixth run. Finally, the CBZ degradation pathways were presented based on the identified intermediates. This research has offered a new strategy of “treating wastes with wastes” to maximize the recycling of electronic wastes to remove emerging pollutants.

研究领域: 环境科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Green and efficient selective lithium extraction from spent lithium-ion batteries using a self-pressurizing-assisted oxidative fixation system

Yong Yan,Yongli Lv,Yuhai Sun,Min Chen,Dan Zhou,Lei Sun,Hai-bin Cheng,Wei-jia Li,Zhi Chen,Cong-Ming Tang,Li Chang,Jun-Qiang Xu

In the recycling of spent lithium batteries, priority lithium extraction is receiving extensive attention because of its prospects and development difficulties. This paper presents a simple, green, and efficient scheme for lithium extraction. In this process, oxidation is the main driving force, and pressure action and ion exchange assist in effectively achieving selective lithium recovery. The experimental results showed that a reasonable configuration of multiple driving forces caused a partial phase transition (cracks appearing) in the layered structure, which ultimately achieved 95.98 % lithium recovery and 94.69 % selectivity. Notably, the lithium-rich leach solution was nearly neutral, and the residue composition was nearly the same as that obtained after cathode charging. Combined with the corresponding characterization results, a mechanism of multiple driving forces for selective lithium extraction is proposed, which will provide a reference for subsequent metal selective recovery.

研究领域: 环境科学 · 材料科学 · 化学工程
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