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.

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, is becoming increasingly important. Spent lithium-ion batteries (LIBs) represent a potential source of raw materials. One possible approach for an optimized recovery of valuable metals from spent LIBs is a combined pyro- and hydrometallurgical process. The generation of mixed cobalt, nickel, and copper alloy and lithium slag as intermediate products in an electric arc furnace is investigated in part 1. Hydrometallurgical recovery of lithium from the Li slag is investigated in part 2 of this article. Kinetic study has shown that the leaching of slag in H2SO4 takes place according to the 3-dimensional diffusion model and the activation energy is 22–24 kJ/mol. Leaching of the silicon from slag is causing formation of gels, which complicates filtration and further recovery of lithium from solutions. The thermodynamic study presented in the work describes the reasons for the formation of gels and the possibilities of their prevention by SiO2 precipitation. Based on these findings, the Li slag was treated by the dry digestion (DD) method followed by dissolution in water. The silicon leaching efficiency was significantly reduced from 50% in the direct leaching experiment to 5% in the DD experiment followed by dissolution, while the high leaching efficiency of lithium was maintained. The study takes into account the preparation of solutions for the future trouble-free acquisition of marketable products from solutions.

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