Enhanced Dissolution of Metal Oxides in Hydroxylated Solvents – Towards Application in Lithium‐Ion Battery Leaching

The recovery of critical metals from spent lithium-ion batteries (LIBs) is rapidly growing. Current methods are energy-intensive and hazardous, while alternative solvent-based strategies require more studies on their 'green' character, metal dissolution mechanism and industrial applicability. Herein, we bridged this gap by studying the effect of dilute HCl solutions in hydroxylated solvents to dissolve Co, Ni and Mn oxides. Ethylene glycol emerged consistently as the most effective solvent, dissolving up to four times more Co and Ni oxides than using aqueous acidic media, attributed to improved chloro-complex formation and solvent effects. These effects had a significant contribution compared to acid type and concentration. The highest Co dissolution (0.27 M) was achieved in 0.5 M HCl in 25 % (v/v) glycerol in water, using less acid and a significant amount of water compared to other solvent systems, as well as mild temperatures (40 °C). This solvent was applied to dissolve battery cathode material, achieving 100 % dissolution of Co and Mn and 94 % dissolution of Ni, following what was concluded to be a mixed mechanism. These results offer a simple alternative to current leaching processes, reducing acid consumption, enhancing atomic efficiency, and paving the way for optimized industrial hydrometallurgical processes leaning to 'greener' strategies.