Effect of hydroxylammonium chloride as a reductant for hydrochloric acid leaching of valuable metals from discarded lithium-ion batteries

Abstract

The use of hydroxylammonium chloride as a reducing agent is proposed to enhance the acid leaching of cathode material from spent lithium-ion batteries. The current study was conducted using real waste from scooter batteries. The main metals found in this cathode material are Mn (43.6%), Li (4.2%), Ni (8.3%) and Co (2.6%), expressed as % w/w. The effect of the initial concentrations of the extracting agent (HCl) and the reducing agent (NH3OHCl) on the extraction yields of the target metals is investigated. The presence of NH3OHCl in HCl solutions exerts a highly effective influence during the initial 15 min of the leaching process, with a complete solubilization of Mn within that timeframe, in contrast to the 20% achieved in its absence. During that period, over 70% of Li is solubilized, while Ni and Co reach maximum solubilities of 7% and 5%, respectively. Extending the contact time to 24 h between the extracting solution and LIB waste enables nearly complete extraction of Ni and exceeds 60% for Co. An analysis of variance was used to identify significant factors to be included in multivariable regressions to predict extraction yields. These regressions are used to carry out a preliminary economic analysis of the leaching process based on gross profit. The optimum outcome is achieved when the extraction is conducted through two consecutive leaching processes. In the first process, 100% Mn and 75% of Li are recovered, while the second process recovers the remaining Li, 96% of Ni, and 60% of cobalt. Additionally, the stoichiometry of the reduction of manganese(IV) by NH3OHCl is studied through the correlation between the gas volume released during the leaching processes and the Mn solubilization reached. This reduction proceeds through two parallel reactions, resulting in the production of N2O and N2. The first of these reactions predominates, exhibiting an estimated selectivity of 87%.