All‐Dry and Scalable Direct Recycling of Spent Ternary Black Mass Toward Long‐Life Ah‑Level Pouch Cell

Abstract

ABSTRACT The direct recycling of spent cathode materials is a promising strategy for a sustainable supply chain but remains challenging for industrial‐sourced cathode black mass due to its complex morphology and heterogeneous impurities. Here, we report an all‑dry and scalable process that directly regenerates spent LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) black mass into high‑performance cathode materials. By integrating plasma‐assisted mechanochemistry with thermal annealing, the process simultaneously refines particle morphology, enhances the relithiation kinetics, and converts trace impurities (Al, Na) into beneficial dopants through plasma‐enabled defluorination and homogeneous incorporation. This enables complete recovery of the layered structure with controlled single‐crystal morphology and preferential (003) facet exposure. The regenerated NCM523 delivers a high specific capacity and long‐term cycling stability, retaining 82.6% of its initial capacity after 300 cycles at a high cut‐off voltage of 4.5 V. Practical scalability of this approach is demonstrated through the batch processing of kilogram‐level black mass, and a 2 Ah pouch cell maintains 97.1% capacity retention over 1000 cycles. This work provides a practical solution for transforming battery black mass into high‑value cathode materials.