Development Of A Hydrometallurgical Path To Recovery Of Critical Materials From Spent Lithium Ion Battery Black Mass - SME Annual Meeting 2022

Since 2019, approximately two dozen international battery recycling companies have been operating at the commercial or pilot scale [1]. However, current process capacity does not exceed 100,000 tons of end-of-life (EOL) lithium-ion batteries (LIB) per year, and the current recycling rate is only about 5% in North America [2-3]. Recycling metals from EOL LIBs is not only essential to waste minimization and environmental stewardship, but also a source of critical materials, which can contribute towards supply chain stabilization. LIB recycling can be roughly divided into three categories: direct recycling, pyrometallurgy, and hydrometallurgy. Direct recycling seeks to retain as much of the manufactured effort with minimum chemical processing [4]. The evolution of battery designs and chemical compositions are challenges to this approach [5-6]. Pyrometallurgical processes are robust and flexible allowing a broad spectrum of batteries with minimum pre-processing requirements. Some of the matrix issues are solved through combustion of some constituents. Smelting is strongly tied to fossil energy and air emissions are a concern. In addition, pyrometallurgical processes are not stand alone, as hydrometallurgical refining normally required to separate and recover the metals of interest (Co, Ni, and Cu) from the produced alloy and Li from the slag [7]. Hydrometallurgical processes can be highly selective and efficient in recovering high purity materials [8]. In general, hydrometallurgical processes are considered cleaner and less costly than high temperature processes [4,9-10]. Extensive chemical consumption and waste generation significantly increase the operating costs and overall environmental impact of the hydrometallurgical processes [11]. Leaching of metals from LIBs is dominated by the mixture of sulfuric acid (1 to 4 M H2SO4) and hydrogen peroxide (1 to 15 wt.% H2O2) [10]. Although organic acids have been tested as lower environmental impact alternatives, the reported pulp density operations are low < 60 g/L [10-11]. For the H2SO4/H2O2 leachates, high leaching efficiencies >90% are reported for Co, Ni, Mn, and Li from cathode materials at temperatures over 40 ⁰C and pulp densities between 30 to 200 g/L [9-10]. H2O2 acts as reducing agent to convert Co+3 and Mn+4 into their soluble forms, Co+2 and Mn+2 [12]. Despite the claims of H2O2 being a clean reducing agent [13], production of H2O2 has significant environmental impacts as determined by life-cycle analyses [13-14]. Moreover, the costs and risks associated with H2O2 transportation and storage cannot be ignored [15].