Environmentally-friendly oxygen-free roasting/wet magnetic separation technology for in situ recycling cobalt, lithium carbonate and graphite from spent LiCoO₂/graphite lithium batteries

Highlights: • The idea of "waste + waste → resources." was used on this study. • Based on thermodynamic analysis, the possible reaction between LiCoO₂ and graphite was obtained. • The residues of oxygen-free roasting are cobalt, lithium carbonate and graphite. • The recovery rate of Co and Li is 95.72% and 98.93% after wet magnetic separation. • It provides the rationale for environmental-friendly recycling spent LIBs in industrial-scale. - Abstract: The definite aim of the present paper is to present some novel methods that use oxygen-free roasting and wet magnetic separation to in situ recycle of cobalt, Lithium Carbonate and Graphite from mixed electrode materials. The in situ recycling means to change waste into resources by its own components, which is an idea of "waste + waste → resources." After mechanical scraping the mixed electrode materials enrich powders of LiCoO₂ and graphite. The possible reaction between LiCoO₂ and graphite was obtained by thermodynamic analysis. The feasibility of the reaction at high temperature was studied with the simultaneous thermogravimetry analysis under standard atmospheric pressure. Then the oxygen-free roasting/wet magnetic separation method was used to transfer the low added value mixed electrode materials to high added value products. The results indicated that, through the serious technologies of oxygen-free roasting and wet magnetic separation, mixture materials consist with LiCoO₂ and graphite powders are transferred to the individual products of cobalt, Lithium Carbonate and Graphite. Because there is not any chemical solution added in the process, the cost of treating secondary pollution can be saved. This study provides a theoretical basis for industrial-scale recycling resources from spent LIBs.