Scalable Direct Recycling of NMC532 From End‐of‐Life Batteries via Physical Separation and Solid‐State Relithiation

Direct recycling retains the structure and value of lithium‐ion battery cathodes, however, most demonstrations rely on manually disassembled cells or chemical purification. A fully integrated, purification‐free direct recycling process for high‐Ni NMC cathodes is reported. Commercial NMC532/graphite pouch cells were sequentially shredded, wet‐sieved, and subjected to electrostatic and magnetic separation to isolate cathode‐rich fractions. Thermal debinding at 500°C removed polyvinylidene fluoride binder, enabling recovery of ≈90 wt% cathode active material (CAM) from aluminium current collectors with simple sieving. The optimal 1–4 mm fraction exhibited >98 wt% purity with <1 wt% total metallic contamination (Al, Cu, Fe). Synchrotron X‐ray fluorescence/μ‐X‐ray absorption near edge structure mapping confirmed residual Cu and Fe as discrete oxide particles, physically isolated from NMC grains. Solid‐state relithiation at 800°C in O 2 , using either commercial or recycled Li 2 CO 3 , restored stoichiometry to Li 1 Ni 0.5 Mn 0.3 Co 0.2 O 2 while preserving spherical secondary particle morphology, providing specific capacities comparable to pristine NMC532 with stable cycling. A cradle‐to‐gate life cycle assessment quantified a product carbon footprint of 2.25 kg CO 2 ‐eq kg −1 for regenerated NMC using recycled Li 2 CO 3 , ≈15% lower than regenerated NMC with virgin Li 2 CO 3 . This study demonstrates a scalable, low‐carbon direct recycling pathway that eliminates chemical purification, maintains high material performance, and is compatible with industrial waste streams.