Intensifying separation of Pb and Sn from waste Pb-Sn alloy by ultrasound-assisted acid leaching: Selective dissolution and sonochemistry mechanism

Abstract

Clean and efficient extraction and separation of precious metals from discarded Pb-Sn alloy is critical to the sustainable utilization of solid waste resources. Dense oxide layer and compact alloy texture in the waste Pb-Sn alloy pose challenges to the effective leaching process. Ultrasonic waves are demonstrated to improve separation efficiency via the favorable physical and chemical effects in solution system. In this study, ultrasound-assisted leaching technology is attempted to rapidly and selectively extract Pb from the waste Pb-Sn alloy, and gives emphasis on ultrasonic electrochemical behaviors. The Eh-pH diagrams of Sn-H2O and Pb-H2O systems were firstly analyzed to lay the selective dissolution foundation. It’s indicated that oxidizing HNO3 lixiviant is suitable to realize the selective separation of Pb. Both Sn and Pb can be dissolved to ionic Sn2+ and Pb2+ in the HNO3 solution. However, Sn2+ rapidly oxidizes to Sn4+ and Sn4+ further hydrolyzes to insoluble SnO2, which will agglomerate on unreacted materials to limit internal metal leaching in conventional leaching process. Due to the vibratory stripping of oxide layer by physical effect of ultrasound, the conventional acid leaching time for Pb extraction can be halved with the ultrasound assistance. About 99.12 % Pb and only 0.1 % Sn are dissolved in ultrasound-assisted leaching under the following optimal parameters: 0.5 mol/L HNO3, leaching temperature of 80 °C, time of 30 min, liquid-to-solid ratio of 20 mL/g, and ultrasound intensity of 0.52 W/cm2. Leaching kinetics of Pb, phase transition, microstructure evolution, Pb-Sn galvanic corrosion and dissolution polarization curve were studied to determine the ultrasonic enhanced dissolution mechanism. Notably, Pb and Sn form a microcorrosion galvanic cell in which Sn acts as a cathode and is protected while the Pb undergoes intensifying corrosion as the anode giving rise to the higher Pb dissolution efficiency. Eventually, it’s suggested that Pb can be rapidly extracted and separated from the waste Pb-Sn alloy during the ultrasound-assisted HNO3 leaching process via the ultrasound physical and chemical effects, especially the sonochemistry aspect of intensified spot corrosion and galvanic corrosion. The proposed ultrasonic electrochemical corrosion in this work were applicable to the extraction of valuable metals from various waste alloys through leaching method.