Optimization of Synergistic Leaching of Valuable Metals from Spent Lithium-Ion Batteries by the Sulfuric Acid-Malonic Acid System Using Response Surface Methodology

Abstract

A new environmentally friendly and economical recycling process for extracting metals from spent lithium-ion batteries (LIBs) using sulfuric acid and malonic acid as leaching agents is proposed. By applying Box-Behnken design (BBD) and response surface methodology (RSM) optimization techniques, the global optimal solution of the maximum leaching rate of metals in spent LIBs is realized. The results show that under the optimal conditions of 0.93 M H2SO4, 0.85 M malonic acid, liquid/solid ratio of 61 g·L–1, the temperature of 70 °C and 5 vol% of 30% H2O2, 99.79% Li, 99.46% Ni, 97.24% Co and 96.88% Mn are recovered within 81 min. The error between the theoretical value and the actual value of the metal leaching rate predicted by the regression model is less than 1.0%. Additionally, the study of leaching kinetics reveals that the leaching process of Li, Ni, Co, and Mn in spent cathode materials was affected by the synergistic effect of interfacial mass transfer and solid product layer diffusion. Economic analysis reveals that evaluation index should be fully considered when formulating recovery processes for different metals. This process can reduce the environmental risks of heavy metal disposal, and allow the reuse of metals recovered from spent LIBs.