Evaluation of hydrometallurgical black mass recycling with simulation-based life cycle assessment

Purpose: The recycling of lithium-ion batteries is an emerging field faced with the challenge of recovering more than the most valuable elements from the batteries. While the literature presents many innovative approaches to the problem, an overview of the technical and environmental prospects of hydrometallurgical black mass recycling remains crucial. The goal was to analyze the impacts of a black mass process flowsheet and suggest ways to further reduce the impacts of battery recycling. 

Methods: The flowsheet was drafted from the literature by combining both state-of-the-art and experimentally demonstrated unit processes by starting with the leaching system, where reductive leaching is performed using only the copper and iron impurities already present in the black mass. The process targeted copper, manganese, cobalt, nickel, and lithium recovery, and three scenarios for manganese recovery were investigated. The flowsheet was simulated using HSC Sim software, and the mass and energy balances were adapted into internally consistent life cycle inventories. The scope was “gate-to-gate” in Europe and CML methodology was used for impact assessment. 

Results and discussion: Assuming that mechanical pre-treatment carries more environmental benefits than burdens, the results indicated that hydrometallurgical black mass recycling had a tentatively lower environmental footprint compared to virgin raw materials in all impact categories except ozone depletion, the results indicated that hydrometallurgical black mass recycling had a tentatively lower environmental footprint compared to virgin raw materials in all impact categories except ozone depletion. Sulfuric acid and neutralizing chemicals were among the most significant contributors to the impacts, and therefore further analysis was conducted based on an experimental study on low acid leaching with a low (< 0.5 M) initial sulfuric acid concentration instead of the baseline 2 M. This reduced the impacts by approximately 30–40% in all categories by decreasing downstream chemical consumption, and more significantly decreased ozone depletion. The challenges and opportunities for further process improvement were also considered. 

Conclusions: The study highlights the importance of process optimization to improve the environmental sustainability of battery chemical production, but also revealed critical research gaps in the experimental literature. Rather than focusing on a single unit process, experimental black mass recycling research should aim at finding solutions that are optimal for the up- and downstream units, such as minimization of aluminum in the black mass and acid consumption.