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

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_0.5Co_0.2Mn_0.3O₂ (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.