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 H 2 SO 4 , 0.85 M malonic acid, and a liquid/ solid ratio of 61 g•L −1 , a temperature of 70 °C and 5 vol % of 30% H 2 O 2 , 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.

Microthermal catalytic aerogenesis of renewable biomass waste using cathode materials from spent lithium-ion batteries towards reversed regulated conversion and recycling of valuable metals

“…The relatively lower E a values indicate that Ni, Co and Mn can be easily leached in this system. 54 Finally, the high value-added product Li 2 CO 3 with high purity (99.99%) was recovered by evaporating the Li-enriched lixivium, and it can be re-used as battery-grade lithium carbonate for the re-fabrication of NCM (see Fig. S6(a)–(b)†), while the transition metal enriched could be directly recovered as Ni x Co y Mn 1− x − y (OH) 2 precursors after adjusting the molar ratio of different transition metals, with reduced alkali consumption due to the reduced acid consumption during leaching.…”

“…The relatively lower E a values indicate that Ni, Co and Mn can be easily leached in this system. 54 Finally, the high value-added product Li 2 CO 3 with high purity (99.99%) was recovered by evaporating the Li-enriched lixivium, and it can be re-used as battery-grade lithium carbonate for the refabrication of NCM (see Fig. S6…”

Carbon neutrality strategies for sustainable batteries: from structure, recycling, and properties to applications

“…Specifically, 99.79% Li, 99.46% Ni, 97.24% Co and 96.88% Mn were recovered in 81 min under the optimal conditions of 0.93 M H 2 SO 4 , 0.85 M malonic acid, liquid/solid ratio of 61 g L −1 , 70 °C, and 5 vol% of 30% H 2 O 2 , respectively. 134 The leaching process was influenced by the synergistic effect of interfacial mass transfer and diffusion of solid product layers.…”

Preparing La-Doped LiAl5O8 from the Electrode Materials of Waste Lithium-Ion Batteries

“…Roasting for 120 min to obtain CoO, the extraction efficiency was up to 98%. Li et al 20 proposed a response surface methodology to optimize the synergistic leaching of valuable metals from waste LIBs by the sulfuric acid−malonic acid system, and 99.79% Li, 99.46% Ni, 97.24% Co, and 96.88% Mn were recovered under optimal conditions. Meanwhile, Wang et al 21 investigated the biodegradable organic methanesulfonic acid to leach valuable metals from waste LiCoO 2 powders, and the leaching efficiencies of Li and Co were achieved at nearly ∼100 and ∼100%.…”