Recycling Process of Spent Alkaline and Zn-C Batteries for the Re-Utilization in Rechargeable Zn-Ion Battery

Abstract

The Zn, Mn and C extraction processes from spent primary batteries and the synthesis of recycled Zn film, MnO2 and MnO2/C for Zn-ion battery application were developed in the project. The Zn, Mn and C extraction process involved the acid leaching of Zn and Mn ions from the spent alkaline and Zn-C battery electrodes in the lab-scale was initially investigated using various leaching conditions. The acid leaching using 0.5-2 M HCl and H2SO4 at ambient temperature providing Zn extraction efficiencies in a range of 72.3-95.3%. By introducing an inexpensive reducing agent namely sodium sulfide (Na2S), sodium metabisulfite (Na2S2O5) or hydrogen peroxide (H2O2) in 2M H2SO4, the Mn extraction efficiency for Mn was increased from 21.9% (with no reducing agent) up to 48.4%, 82.8% and 98.9%, respectively. The upscale leaching study was subsequently performed in a 100-L pilot scale reactor demonstrated the Zn and Mn extraction efficiencies of 71% and 65%, respectively. Using the leaching solutions from the upscale hydrometallurgical route, Zn-film fabrication via electrodeposition process, and the MnO2 and MnO2/C synthesis via hydrothermal techniques were performed. Additionally, the one-step synthesis of MnO2/C via one-step hydrothermal method with no acid leaching was also explored in this study. The recycled Zn, MnO2, MnO2/C and C residual were subsequently used as the anode and cathode main components in the CR2032 and pouch-cell rechargeable Zn-ion batteries. The recycled MnO2 and MnO2/C provided similar performance as the commercial products, which indicating the recycled MnO2, MnO2/C could be effectively utilized in the Zn-ion battery, while the utilization of recycled Zn-film provided slightly lower performance compared to that of the commercial Zn foil.