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Molecules 2017, 22, 403 6 of 21 and Fe accumulate inside the slag and are disposed. The organic cell components including the electrolyte are incinerated. In the following hydro-metallurgical step, the alloy fraction is separated and refined for re-utilization [116]. With the growing market for xEVs, the amount of spent LIBs will drastically increase. Considering several hundred kilograms of LIB cell material per car and taking into account that similar cell chemistries are used by the manufacturers, a continuous material flow is created. Therefore, a more holistic recycling process can be applied (Figure 4), including the recovery of the electrolyte [117]. This mechanical-hydrometallurgical process aims to meet the demands of the EU directive and therefore the utilization of most cell materials from a LIB. The deep discharged (by external resistance or power) battery packs are dismantled to the individual cell level and shredded in an inert atmosphere [108,114,118]. The electrolyte evaporated during this first step is collected by condensation. The electrolyte remaining in the shredded material is subject to three possible recovery methods: (i) a thermal drying step with the disadvantage of losing the conducting salt, which is the most costly component of the electrolyte; (ii) application of supercritical CO2 in a static setup; and (iii) supercritical CO2 in a flow-through setup with co-solvents for the recovery of the whole electrolyte including the conducting salt. The latter two setups will be discussed in Section 6, here we concentrate on method (i): the shredded material is further processed by removing iron parts via a magnetic separation tool and then the electrode material is parted from the separator by air flow. The binder in the electrodes is removed by heating up to 400–600 °C which additionally causes the detachment of the current collectors from the active material particles. The graphite anode material and the copper and aluminum current collectors are taken out of the process and lithium is leached out of the cathode material, while the active material is dissolved in an acidic mixture. Several approaches are carried out to separate the heavy metals from each other: complexing agents such as di(2,4,4,trimethylpentyl)phosphinic acid [119]; or leaching with oxalate [120], ascorbic [121], citric [122] or concentrated acids [123–125]. However, biological approaches are also investigated [126]. The performance of the resynthesized cathode and anode material was reported by electrochemically and analytically characterized [127,128]. Figure 4. The mechanical-hydrometallurigcal “LithoRec II” recycling process. It was reproduced from reference [127], with permission from John Wiley & Sons 2016. scCO2: supercritical carbon dioxide.PDF Image | CO2 for Recycling and Sample Preparation of Lithium Ion Battery
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