Flux Upcycling of Degraded Layered Cathodes to LiNi _x Mn _y Co _z O ₂ (NMCs) with Gradient Transition Metal Distribution

Abstract The rising demand for lithium‐ion batteries (LIBs) has intensified the need for efficient recycling methods to address both supply chain constraints and environmental impacts. Direct upcycling, distinguished by its ability to achieve both the structural and compositional integrity of cathode materials, has gained prominence as a sustainable alternative to conventional pyrometallurgical and hydrometallurgical processes. However, the current direct upcycling methods are typically limited by incorporating Li and/or Ni, significantly constraining the adaptability across diverse LiNi x Mn y Co z O 2 (NMCs). In this study, a versatile molten salt approach is reported that expands the scope of direct upcycling by enabling simultaneous incorporation of Li, Ni, and Mn. This methodology facilitates flexible conversion among diverse NMC compositions, including non‐stoichiometric Co/Mn systems such as upcycling degraded LiCoO 2 (D‐LCO), LiNi 1/3 Mn 1/3 Co 1/3 O 2 (D‐NMC111), LiNi 0.8 Mn 0.1 Co 0.1 O 2 (D‐NMC811) to surface Mn enriched NMC111, LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532), and NMC811, respectively. The gradient transition metal distribution in upcycled products, characterized by Mn‐enriched outer layers and Co/Ni‐enriched cores enhances the interfacial stability of NMC cathodes, addressing critical challenges in long‐term performance and structural integrity. These results highlight the potential of flux methods for advancing the upcycling of spent cathodes and producing high‐performance materials for next‐generation LIBs applications.