Open Access Article
This Open Access Article is licensed under a Creative Commons Attribution-Non Commercial 3.0 Unported LicenceScalable Upcycling of Spent LiNixCoyMn1−x−yO2 to Single-Crystal Ni-Rich Cathodes Using a Low-Cost, Multifunctional Ni Salt
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Xiaolu Yu , Greta Feague , Sicen Yu , Varun Gupta , Hongpeng Gao , Wei Li , Maura Appleberry , Ping Liu , Jiao Lin and Zheng Chen
First published on 15th September 2025
Abstract
The urgent need to recycle spent lithium-ion batteries (LIBs) is driven by the dual pressure of raw material scarcity and ecological sustainability. Closed-loop recycling of spent LIBs not only recovers valuable materials but also minimizes harmful environmental impacts, offering an efficient strategy to the increasing demand for critical resources. Here, we introduce a thermally-driven selective upcycling process that extracts lithium from spent polycrystalline LiNi0.33Co0.33Mn0.33O2 (NCM111) using NiSO4. This process subsequently converts the residual materials into single-crystal Ni-rich cathodes with minimal input of nickel and lithium. We demonstrate that both chemically delithiated NCM111 and spent NCM111 black mass can be upgraded in terms of composition, structure, and electrochemical performance to match the pristine LiNi0.6Co0.2Mn0.2O2 (NCM622) and LiNi0.8Co0.1Mn0.1O2 (NCM811). Life-cycle analysis reveals that this closed-loop selective upcycling approach significantly reduces energy consumption and greenhouse gas emissions, offering superior economic and environmental advantages over conventional hydrometallurgical, pyrometallurgical, and cathode production methods. This work establishes a foundation for cost-effective upcycling strategies, advancing the sustainable development of NCM materials and selective recovery for LIBs.