Efficient Recycling of Spent LiCoO₂ Cathodes Via Confined Pore-Assisted Simplified Direct Carbothermic Reduction Without External Reducing Agents

Abstract

As demand for lithium-ion batteries increases, the supply of materials is increasingly constrained by their geographical concentration. This has spurred significant research into recycling spent batteries to enhance resource circulation. Currently, commercially applied recycling methods (such as pyrometallurgy and hydrometallurgy) face environmental and economic challenges, including waste acid and gas generation, high-temperature heat treatment, and operational complexity. A promising alternative is the carbothermic reduction process, which operates at lower temperatures, minimizing costs and environmental emissions. However, this method still requires large quantities of external reducing agents. Therefore, this study aims to introduce a simplified direct carbothermic reduction (SDCR) process. The SDCR process leveraged carbon conductive materials and organic binders within the electrode as reducing agents. Additionally, the high compaction state created a conducive environment for reducing gases, promoting efficient reduction and material recovery. This approach reduces the reliance on external reducing agents and streamlines the re-upcycling process, making it commercially viable.

Keywords

carbothermic reduction / closed-loop recycling / lithium-ion batteries / simplified direct carbothermic reduction / spent cathode material

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2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.