High-yield recycling and recovery of copper, indium, and gallium from waste copper indium gallium selenide thin-film solar panels

Abstract

A separation process for Cu, In, Ga, and Se (CIGS)-based thin-film solar panels is proposed in this study. Initially, the separation process, by peeling off the panels in a layer-by-layer manner, was achieved by utilizing the different thermal strains of materials inside the CIGS solar panels. Subsequently, the recovery process was performed by annealing the CIGS layers for the removal of Se, and then leaching was performed with nitric acid, followed by the individual extraction of valuable metals. The pH values, concentrations of extractant, stripping agents, organic-aqueous ratios, and reaction time were investigated in detail to optimize the separation conditions for Cu, In, and Ga. First, In was extracted using di-(2-ethylhexyl) phosphoric acid into the organic phase, while Cu and Ga remained in the aqueous phase, by controlling the extraction conditions. After the extraction of In, Ga was extracted using the same extraction agent under different conditions, and nearly pure Cu remained in the residual aqueous solution. Ammonium hydroxide was added to three solutions to form metal hydroxide precipitates. Under the optimal conditions, a recovery rate of >90% could be achieved for In, Ga, and Cu. Furthermore, all as-formed hydroxides were recycled and converted into metal oxides with a purity of >99% by calcination. These findings can provide a pathway for the effective recycling and recovery of Cu, In, and Ga from waste CIGS thin-film solar panels. • A facile and practical method to separate and recover valuable metals respectively from the real commercial thin-film solar panel was demonstrated. • A novel and low-cost physical separation process was induced to peer off the solar panel layer by layer via the extremely low-temperature liquid nitrogen treatment. • An extraction and stripping process was designed to separate Cu, In, and Ga from a complicated multi-element system individually. • Highly pure valuable metal oxides were recovered as the final products, establishing a possible curcular economy model for waste solar panel recycling and recovery.