Ultrasound-assisted sustainable recycling of valuable metals from spent Li-ion batteries via optimisation using response surface methodology

Abstract

In this study, the use of response surface methodology was proposed to optimise a novel green leaching process for recovering Li and Co from spent lithium-ion batteries (LIBs), assisted by ultrasonic irradiation and gluconic acid. This work investigated various parameters such as temperature, time, gluconic acid concentration, and ultrasound power (US power). To enhance the interpretability and optimisation of experimental data on metal leaching, the central composed design (CCD) was utilised to establish a predictive model. A statistical analysis using the analysis of variance (ANOVA) test was conducted to validate the quadratic model and determine the significant operating parameters, indicated by p-values (< 0.05). The model exhibited Adj R2 values of 0.98 for Li leaching and 0.96 for Co leaching, respectively. To confirm the results, additional characterisations of the solid residues were performed using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transformation infrared spectrometer (FT-IR/NIR). The leach liquor was subjected to precipitation and crystallisation methods to recover Li and Co. The purity of Li2CO3 and Co3O4 was confirmed to be ≥ 99% and ≥ 98.8%, respectively, through ICP-OES analysis. Finally, the recovered Li2CO3 and Co3O4 were utilised in a 1:1 molar ratio for regenerating new LiCoO2 cathode materials using a solid-state method. The resulting cathode materials exhibited high purity (≥ 99.43%) as confirmed by ICP-OES analysis. The obtained results demonstrate that ultrasound irradiation significantly enhanced the dissolution of metal oxides within the mixture. Furthermore, gluconic acid exhibited a dual function, acting as both an oxidising and reducing agent. Consequently, this process presents a promising and sustainable alternative for recycling valuable metals from spent LIBs.