A Novel Pyrometallurgical Recycling Process for Lithium-Ion Batteries and Its Application to the Recycling of LCO and LFP

The bottleneck of recycling chains for spent lithium-ion batteries (LIBs) is the recovery of valuable metals from the black matter that remains after dismantling and deactivation in pretreatment processes, which has to be treated in a subsequent step with pyrometallurgical and/or hydrometallurgical methods. In the course of this paper, investigations in a heating microscope were conducted to determine the high-temperature behavior of the cathode materials lithium cobalt oxide (LCO—chem., LiCoO2) and lithium iron phosphate (LFP—chem., LiFePO4) from LIB with carbon addition. For the purpose of continuous process development of a novel pyrometallurgical recycling process and adaptation of this to the requirements of the LIB material, two different reactor designs were examined. When treating LCO in an Al2O3 crucible, lithium could be removed at a rate of 76% via the gas stream, which is directly and purely available for further processing. In contrast, a removal rate of lithium of up to 97% was achieved in an MgO crucible. In addition, the basic capability of the concept for the treatment of LFP was investigated whereby a phosphorus removal rate of 64% with a simultaneous lithium removal rate of 68% was observed.