Lithium ion battery active material dissolution kinetics in Fe(II)/Fe(III) catalyzed Cu-H2SO4 leaching system

The use of lithium-ion batteries as energy storage in portable electronics and electric vehicles is increasing rapidly, which involves the consequent increase of battery waste. Hence, the development of reusing and recycling techniques is important to minimize the environmental impact of these residues and favor the circular economy goal. This paper presents experimental and modeling results for the hydrometallurgical treatment for recycling LiCoO2 cathodes from lithium-ion batteries. Previous experimental results for hydrometallurgical extraction showed that acidic leaching of LiCoO2 particles produced a non-stoichiometric extraction of lithium and cobalt. Furthermore, the maximum lithium extraction obtained experimentally seemed to be limited, reaching values of approximately 65–70%. In this paper, a physicochemical model is presented aiming to increase the understanding of the leaching process and the aforementioned limitations. The model describes the heterogeneous solid–liquid extraction mechanism and kinetics of LiCoO2 particles under a weakly reducing environment. The model presented here sets the basis for a more general theoretical framework that would describe the process under different acidic and reducing conditions. The model is validated with two sets of experiments at different conditions of acid concentration (0.1 and 2.5 M HCl) and solid to liquid ratio (5 and 50 g L−1). The COMSOL Multiphysics program was used to adjust the parameters in the kinetic model with the experimental results.

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“…The dissolution reaction of LiCoO 2 particles in acid media, expressed as a redox half-reaction, can be described as [25]:…”

Section: Physicochemical Modelmentioning

confidence: 99%

Hydrometallurgical Extraction of Li and Co from LiCoO2 Particles–Experimental and Modeling

et al. 2020

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“…In many of the currently operational hydrometallurgical recycling plants, these elements are considered as impurities that complicate the leaching process [4]. For this reason, research efforts have been made to better optimize leaching operations for mixed feeds involving Fe, Cu, and Al [16,17]. However, as Cu, Al, and Fe are significantly lower in economic value compared to the elements in the electrodes, recovering them by mechanical unit operations would be preferable over the relatively expensive chemical methods.…”

Section: Introductionmentioning

confidence: 99%

Worth from Waste: Utilizing a Graphite-Rich Fraction from Spent Lithium-Ion Batteries as Alternative Reductant in Nickel Slag Cleaning

et al. 2021

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One possible way of recovering metals from spent lithium-ion batteries is to integrate the recycling with already existing metallurgical processes. This study continues our effort on integrating froth flotation and nickel-slag cleaning process for metal recovery from spent batteries (SBs), using anodic graphite as the main reductant. The SBs used in this study was a froth fraction from flotation of industrially prepared black mass. The effect of different ratios of Ni-slag to SBs on the time-dependent phase formation and metal behavior was investigated. The possible influence of graphite and sulfur contents in the system on the metal alloy/matte formation was described. The trace element (Co, Cu, Ni, and Mn) concentrations in the slag were analyzed using the laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) technique. The distribution coefficients of cobalt and nickel between the metallic or sulfidic phase (metal alloy/matte) and the coexisting slag increased with the increasing amount of SBs in the starting mixture. However, with the increasing concentrations of graphite in the starting mixture (from 0.99 wt.% to 3.97 wt.%), the Fe concentration in both metal alloy and matte also increased (from 29 wt.% to 68 wt.% and from 7 wt.% to 49 wt.%, respectively), which may be challenging if further hydrometallurgical treatment is expected. Therefore, the composition of metal alloy/matte must be adjusted depending on the further steps for metal recovery.

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“…Although lithium does not represent a critical metal, its recovery, especially regarding future battery systems, where lithium will be manifested as an indispensable cathode component, becomes essential. In the field of battery recycling, research projects have been carried out for several years dealing with both single and combined mechanical, pyrometallurgical and hydrometallurgical processes as well as pyrolysis to recover battery components [5,10,11,[13][14][15][16][17][18][19][20][21][22][23]. However, the focus is set mainly on critical and valuable metals, which is the reason why lithium as a component has not been sufficiently considered [24].…”

Section: Introductionmentioning

confidence: 99%

A Combined Pyro- and Hydrometallurgical Approach to Recycle Pyrolyzed Lithium-Ion Battery Black Mass Part 1: Production of Lithium Concentrates in an Electric Arc Furnace

Sommerfeld¹,

Vonderstein²,

Dertmann³

et al. 2020

Metals

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Due to the increasing demand for battery raw materials such as cobalt, nickel, manganese, and lithium, the extraction of these metals not only from primary, but also from secondary sources like spent lithium-ion batteries (LIBs) is becoming increasingly important. One possible approach for an optimized recovery of valuable metals from spent LIBs is a combined pyro- and hydrometallurgical process. According to the pyrometallurgical process route, in this paper, a suitable slag design for the generation of slag enriched by lithium and mixed cobalt, nickel, and copper alloy as intermediate products in a laboratory electric arc furnace was investigated. Smelting experiments were carried out using pyrolyzed pelletized black mass, copper(II) oxide, and different quartz additions as a flux to investigate the influence on lithium-slagging. With the proposed smelting operation, lithium could be enriched with a maximum yield of 82.4% in the slag, whereas the yield for cobalt, nickel, and copper in the metal alloy was 81.6%, 93.3%, and 90.7% respectively. The slag obtained from the melting process is investigated by chemical and mineralogical characterization techniques. Hydrometallurgical treatment to recover lithium is carried out with the slag and presented in part 2.

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Lithium ion battery active material dissolution kinetics in Fe(II)/Fe(III) catalyzed Cu-H2SO4 leaching system

Cited by 40 publications

References 25 publications

Hydrometallurgical Extraction of Li and Co from LiCoO2 Particles–Experimental and Modeling

Hydrometallurgical Extraction of Li and Co from LiCoO2 Particles–Experimental and Modeling

Worth from Waste: Utilizing a Graphite-Rich Fraction from Spent Lithium-Ion Batteries as Alternative Reductant in Nickel Slag Cleaning

A Combined Pyro- and Hydrometallurgical Approach to Recycle Pyrolyzed Lithium-Ion Battery Black Mass Part 1: Production of Lithium Concentrates in an Electric Arc Furnace

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