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therefore difficult to separate from each other. Research at Worcester Institute of Technology uses the mixture without separation, adding suf- ficient virgin materials to obtain relative propor- tions appropriate for production of a desired re- manufactured cathode formulation [19]. For most cathode chemistries, the constituents in the solu- tion have some intrinsic value, and their recovery after leaching makes economic sense. However, for some cathode materials, such as lithium iron phosphate (LFP) and lithium manganese oxide (LMO), the constituent value is so low that hy- drometallurgy does not pay. Direct recovery of LFP could be economical, and representatives from BYD Co. claimed that its achievement in China, but could provide no details [20]. Direct recovery of LFP has been reported in the litera- ture [21]. The positive side of breaking down the struc- ture by hydrometallurgy is that the outputs are ge- neric products, and are not specific to a particular cathode structure, and can therefore be used as in- puts to produce a variety of new products. Out- puts of direct recycling, however, are assumed to retain a specific, well-defined structure. Although retention of structure can be considered an ad- vantage, it poses a limitation, because (unless cathode mixtures are found to be useful) inputs to direct recycling must be segregated by cathode type, or the output will be a mixture of signifi- cantly reduced value. No effective and economic separation technology for cathode material has been proven for use before or after recycling, alt- hough a magnetic separation method has been pa- tented [22]. Therefore, most businesses entering the recycling arena today are proposing variants of hydrometallurgical processes. Retention of structure also means that the formulation recov- ered at the end of vehicle life and battery second- life is likely to be on the order of 15 years old, and may have been supplanted be newer materi- als. However, prompt scrap would avoid that po- tential difficulty and would make excellent feed- stock for a pilot plant demonstration of direct re- cycling. Reuse of prompt scrap provides an op- portunity for manufacturers to gain practice in the use of reclaimed material and eliminates a poten- tial disposition cost. Although most of the discussion so far has concerned recovery of cathode material and metal foils, it is also possible to recover anode and even electrolyte using low-temperature processes. Both are, of course, burned in a smelter, supply- ing some of the process fuel. Separators are also burned in a smelter. No process has been pro- posed for recovering separators because their value lies in their specialized form factor (thin po- rous film), which would be lost in any processing. The polymeric raw materials could be recovered, but their value is low. Recovery of anode material using simple physical processes has been demonstrated as part of direct recycling; anode material is less valua- ble than cathode, but must be separated out to ob- tain usable cathode material. Different methods of separating the black mass into anode and cath- ode fractions have been reported, including froth flotation and gravity separation using dense liq- uids [23][24]. Anode material could also be re- covered with hydrometallurgical processes. Ac- ids do not dissolve graphite, which would remain as a solid while the cathode dissolves. The mate- rial could then be recovered by filtration, but its quality becomes an issue. As can be seen in Fig. 6, anode material from spent cells may be coated with a solid-electrolyte interphase (SEI) layer and the particle structure may be degraded. Such material has been shown to perform well in recycled cells, but potential concerns exist about performance after repeated recycling. There are similar concerns about cathode material. Figure 7 (courtesy of Daniel Abraham, Argonne) shows lithium nickel/cobalt/aluminum oxide (NCA) particles before (left) and after (right) 6000 cy- cles. Particle separation and planar defects are visible. The cell from which the aged particle was taken showed ~33% capacity fade, but some per- formance could possibly be restored through treatment. Recovery of electrolyte, including the lithium salts, by extraction of breached cells with super- critical CO2 has been demonstrated [25]. Alt- hough the recovered electrolyte performed well in recycled cells, the process is not believed to be cost-effective. Solvent extraction is also possible, but the low value and expected contamination by degradation products has limited investigation of electrolyte recovery. Interest may increase when large volumes of material are actually being pro- cessed. 6PDF Image | Lithium-Ion Battery Recycling Processes
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