Advances in Recycling and Functionalization of Graphite from Spent Lithium-Ion Battery Anodes
Received Date:2025-08-29
Revised Date:2025-12-01
Accepted Date:2025-12-03
DOI:10.20078/j.eep.20251204
Abstract:With the rapid expansion of the electric vehicle industry, the quantity of spent lithium-ion batteries has witnessed a s... Open+
Abstract:With the rapid expansion of the electric vehicle industry, the quantity of spent lithium-ion batteries has witnessed a sharp increase, which underscores the significance of recycling and reutilizing spent graphite anodes for sustainable development. Although spent graphite retains a relatively stable layered framework after cycling, it also exhibits structural defects, residual electrolyte components, and other surface contaminants. These issues limit its direct reuse in new batteries but create opportunities for targeted regeneration and functional transformation. This review provides a comprehensive overview of recent advances in the repair, regeneration, and functional utilization of graphite anodes from spent lithium-ion batteries. Repair and regeneration aim to restore the electrochemical activity of degraded graphite by removing impurities, repairing structural defects, and reconstructing the electrode-electrolyte interface. Low-to-medium-temperature graphitization, enabled by the introduction of transition metal catalysts that reduce the migration energy barrier of carbon atoms, allows the graphitization process to proceed at lower temperatures and with reduced energy consumption. Surface treatments focus on constructing protective coatings on damaged graphite surfaces to cover defect regions, improve structural integrity, and stabilize the electrode-electrolyte interface, thereby suppressing undesired side reactions. Rapid heating treatments, such as microwave irradiation and Joule heating, generate localized high temperatures within seconds, enabling efficient removal of surface residues and repair of near-surface defects in an energy-saving and environmentally friendly manner. Functional utilization leverages the intrinsic defects, porous structures, and the ability of spent graphite to incorporate heteroatoms or metals. By tailoring surface morphology and introducing functional elements, spent graphite can be converted into advanced functional materials for diverse applications. Defect sites and residual heteroatoms can serve as catalytic centers for electrocatalysis and pollutant degradation, while the engineered porous structures and surface functional groups enhance the adsorption of heavy metals and organic contaminants in aqueous environments. Furthermore, strategies such as defect engineering, heteroatom doping, and composite formation enhance ionic transport and capacitive performance, facilitating the development of porous carbons, doped graphene, and graphite-based composites for supercapacitors as well as sodium-ion and potassium-ion batteries. From an environmental and economic perspective, graphite regeneration and utilization provide distinct advantages over conventional recycling methods. Repair and regeneration reduce greenhouse gas emissions and minimize secondary pollution, while functional utilization mitigates waste and generates economic value by producing functional materials with ecological benefits. Despite notable progress, large-scale recycling of spent graphite remains challenging due to high energy consumption, complex processing steps, and the limited availability of efficient, scalable technologies. In addition, the diversity of waste sources complicates the establishment of standardized pretreatment and regeneration procedures. Future research should focus on developing intelligent and universal recycling technologies, along with the construction of integrated closed- and open-loop pathways, to achieve resource-efficient, environmentally compatible, and value-added reutilization of spent graphite. The coordinated implementation of these strategies is expected to enhance efficiency, reduce costs, and maximize the resource potential of spent graphite, thereby supporting a sustainable and circular lithium-ion battery industry. Close-
Authors:
- MA Xiaofan1,2
- KONG Lingchao3
- HU Kailong1,2,*
- ZHANG Jialiang4,*
Units
- 1. Zhongyuan Key Metals Laboratory
- 2. School of Materials Science and Engineering, Harbin Institute of Technology Shenzhen
- 3. Shenzhen Xinmao New Energy Technology Co., Ltd.
- 4. School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing
Keywords
- Spent lithium ion batteries
- Graphite
- Regeneration
- Repair
- Functional materials
Citation