Abstract
The rapid growth of electric vehicles and grid-scale storage has intensified global demand for critical battery metals while simultaneously increasing end‑of‑life lithium-ion battery waste. To support secure, low‑carbon, and resilient supply chains, industry requires recycling technologies that combine high recovery, predictable performance, and reduced environmental burden. This work evaluates supercritical CO2 extraction (SCFE) as an industrially practical route for recovering lithium, cobalt, nickel, and manganese from real NMC111 black mass, positioning CO2 as both a processing medium and a strategic enabler in critical‑materials recovery. The SCFE process uses chelating and reducing agents dissolved in supercritical CO2 to selectively extract target metals under moderate conditions. Under optimized conditions, metal recoveries reached 93% Co, 93% Ni, 98% Mn, and 73% Li, demonstrating yields competitive with hydrometallurgy while substantially reducing aqueous waste and chemical consumption. These process conditions align with existing industrial supercritical equipment designs and support safe, closed‑loop solvent operation. To enable scale‑up and process control, a predictive kinetic framework was developed by integrating Sovová’s broken‑and‑intact‑cell (BIC) model with the shrinking‑core model. The BIC model reproduced extraction behavior with <1.1% deviation, indicating a Type A regime governed by an initial rapid surface extraction followed by diffusion‑limited intraparticle transport. From an industrial perspective, the use of nonflammable supercritical CO2 improves safety, reduces solvent recovery costs, and minimizes corrosion risk, extending equipment lifetime. The validated modeling framework supports accurate equipment sizing, feedstock variability management, and operational forecasting. This work provides an industry‑aligned, mechanistically grounded foundation for deploying supercritical CO2 extraction at commercial scale, strengthening critical‑materials supply chains and enabling circular‑economy strategies for strategic battery metals.