Li-Distribution in Compounds of the Li2O-MgO-Al2O3-SiO2-CaO System—A First Survey

The recovery of critical elements in recycling processes of complex high-tech products is often limited when applying only mechanical separation methods. A possible route is the pyrometallurgical processing that allows transferring of important critical elements into an alloy melt. Chemical rather ignoble elements will report in slag or dust. Valuable ignoble elements such as lithium should be recovered out of that material stream. A novel approach to accomplish this is enrichment in engineered artificial minerals (EnAM). An application with a high potential for resource efficient solutions is the pyrometallurgical processing of Li ion batteries. Starting from comparatively simple slag compositions such as the Li-Al-Si-Ca-O system, the next level of complexity is reached when adding Mg, derived from slag builders or other sources. Every additional component will change the distribution of Li between the compounds generated in the slag. Investigations with powder X-Ray diffraction (PXRD) and electron probe microanalysis (EPMA) of solidified melt of the five-compound system Li2O-MgO-Al2O3- SiO2-CaO reveal that Li can occur in various compounds from beginning to the end of the crystallization. Among these compounds are Li1−x(Al1−xSix)O2, Li1−xMgy(Al)(Al3/2y+xSi2−x−3/2y)O6, solid solutions of Mg1−(3/2y)Al2+yO4/LiAl5O8 and Ca-alumosilicate (melilite). There are indications of segregation processes of Al-rich and Si(Ca)-rich melts. The experimental results were compared with solidification curves via thermodynamic calculations of the systems MgO-Al2O3 and Li2O-SiO2-Al2O3.