Organic acid-based linear free energy relationship models for green leaching of strategic metals from spent lithium-ion batteries and improvement of leaching performance

Abstract

Water-soluble organic acids (e.g., acetic acid, acrylic acid, and ascorbic acid), as green leachants, have been applied to leach strategic metals (Ni, Li, Mn, and Co) from spent lithium-ion batteries (LIBs). Organic acid-based linear free energy relationship models were developed and simulated to predict the feasibility of the leaching efficiency for each of the strategic metals based on in silico calculated descriptors. The developed models, with accuracy (R2) of 0.747–0.831, reveal that hydrogen bond acidity of organic acids promotes the leaching efficiency, whereas molecular volume or excess molar refraction inhibits the efficiency. Furthermore, toxicity (lethal dose 50%) of organic acids was discussed along with the predicted leaching efficiency to explore more green and efficient organic acids. Considering both toxicity and leaching efficiency, citric acid was selected as a green and efficient leachant. To more improve the leaching performance (rate and efficiency) of citric acid, glucose as a green reductant and microwave treatment were additionally applied. Under the selected conditions, the leaching efficiencies after 1 h for Ni, Li, Mn, and Co were enhanced up to 98.3%, 99.1%, 98.7%, and 97.7%, respectively.