Regeneration of raw materials for aluminum electrolysis from spent carbon anodes via a closed-loop environmentally-friendly process based on aluminum–fluorine complexation

Spent carbon anode (SCA) discharged from the aluminum electrolysis industry is an unavoidable solid waste with an estimated production of 700 kilotons in 2021, which has been widely identified as the hazardous solid waste. A new two-stage leaching scheme comprising an aluminum salt leaching and an alkali leaching has been investigated in this study, by which valuable elements have been extracted from SCA. Effect of reaction conditions on the first-stage aluminum salt leaching process was investigated in detail. Under the optimal leaching conditions, the leaching rates of F, Na, and Al reached 98.00%, 94.94%, and 93.94%, respectively, and the recovered carbon purity was 85.84%. The fluorine recovery route was followed by the preparation of aluminum hydroxyfluoride precursor, namely Al2F3.24(OH)2.76 1.65H2O, through the mixing of two filtrates. Then thermogravimetry-differential scanning calorimetry (TG-DSC) curves were used to explore its calcination temperature point in detail. The final product was obtained as a mixture of AlF3 and Al2O3 with 95.94% purity. The characterization results showed that the calcined product was very similar to the commercial aluminum fluoride. Finally, the neutralized filtrate will be prepared by freezing and crystallizing Na2SO4, and the crystallized solution will be returned to the aluminum salt leaching process for recycling, which is the promise of green, recyclable, and high-value technology for realizing the detoxification of SCA and its subsequent utilization.