Two-Stage Organic Acid Leaching of Industrially Sourced LFP- and NMC-Containing Black Mass

Abstract

Over the next 5–10 years, the feedstock to lithium-ion battery recycling facilities will shift from Co- and Ni-rich chemistries to lower-value battery chemistries, such as lithium iron phosphate (LFP). Traditional recycling processes use toxic and corrosive inorganic acids for leaching, generating toxic waste streams. The low-value feedstocks will be LFP-rich with contamination from lithium cobalt oxide (LCO) and lithium–nickel–manganese–cobalt oxide (NMC) battery chemistries. Overall, the lower-value feedstock coupled with the need to reduce environmentally damaging waste streams requires the development of robust, green leaching processes capable of selectively targeting the LFP and LCO/NMC battery chemistries. This research concluded that a first-stage oxalic acid leach could selectively extract Al, Li, and P from the industrially sourced LFP-rich black mass. When operating at the optimal conditions (0.5 M oxalic acid, 5% solids, pH 0.8, and an agitation speed of 600 rpm), >99% of the Li and P and >97% of the Al were selectively extracted after 2 h, while Mn, Fe, Cu, Ni, and Co extractions were kept relatively low, namely, at 19%, <3%, <1%, 0%, and 0%. This research also explored a second-stage leach to treat the first-stage leach residue using ascorbic acid, citric acid, and glycine. It was concluded that when leaching with glycine (30 g/L glycine, a temperature of 40 °C, an agitation speed of 600 rpm, and 2% solids at pH 9.6), that >97% of the Co, >77% of the Ni, and 41% of the Mn were extracted, while the co-extraction percentages of Cu, Fe, and Al were <27%, <4%, and <2%.