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.
Sita et al. (Wed,) studied this question.