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

Pengwei Li; Shao-Hua Luo; Faxian Su; Lin Zhang; Shengxue Yan; Xuefei Lei; Wenning Mu; Qing Wang; Yahui Zhang; Xin Liu; Pengqing Hou

doi:10.1021/acsami.1c23258

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

ACS Appl Mater Interfaces. 2022 Mar 9;14(9):11359-11374. doi: 10.1021/acsami.1c23258. Epub 2022 Feb 22.

Authors

Pengwei Li^{1

2}, Shao-Hua Luo^{1

3

4

2

5}, Faxian Su^{4

2}, Lin Zhang^{1

2}, Shengxue Yan^{1

2}, Xuefei Lei^{1

4

2

5}, Wenning Mu^{1

4

2

5}, Qing Wang^{1

4

2}, Yahui Zhang^{1

4

2}, Xin Liu^{1

4

2}, Pengqing Hou^{4

6}

Affiliations

¹ School of Materials Science and Engineering, Northeastern University, Shenyang 110819, PR China.
² Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province, Qinhuangdao 066004, PR China.
³ State Key Laboratory of Rolling and Automation, Northeastern University, Shenyang 110819, PR China.
⁴ School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, PR China.
⁵ Qinhuangdao Laboratory of Resources Cleaner Conversion and Efficient Utilization, Qinhuangdao 066004, PR China.
⁶ School of Materials Science and Engineering, Anhui University of Technology, Maanshan 243002, PR China.

PMID: 35191662
DOI: 10.1021/acsami.1c23258

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, and a liquid/solid ratio of 61 g·L^-1, a 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.

Keywords: kinetics; leaching; recycle; response surface methodology; spent lithium-ion batteries.