废旧锂离子电池低共熔溶剂回收研究进展

Research progress on recovery of deep eutectic solvent from spent lithium-ion batteries

摘要

随着新能源产业的快速迭代，锂离子电池（LIBs）已广泛应用于电动汽车、储能设备等领域，但受限于滞后的回收模式，全球废旧 LIBs 年产生量已突破百万吨. 废旧 LIBs 中含有的钴、镍、锂等稀缺金属及电解液、粘结剂等有毒成分，若处置不当易造成资源浪费与土壤、水体污染，因此废旧 LIBs 的高效回收再利用已成为保障资源安全、推动“双碳”目标实现的战略重点. 低共熔溶剂（DESs）作为一类由氢键供体与受体按特定比例混合形成的新型绿色溶剂，凭借环境相容性优异、可回收性强、理化性质可调及对正极金属氧化物溶解能力突出等优势，逐步替代传统有毒挥发性溶剂，在废旧 LIBs 回收领域展现出显著的实用价值与经济可行性. 本文系统梳理了近年来 DESs 回收废旧 LIBs 的研究现状，重点阐述了电池正极材料中有价金属的提取机制及核心机理. 同时，深入分析了不同 DESs 体系的分离原理，厘清其核心浸出机理差异. 在此基础上，进一步探讨了当前 DESs 回收技术面临的瓶颈问题，最后，对未来高效、绿色、可持续的 DESs 回收废旧 LIBs 技术路径进行展望，为该领域的后续研究与工程化应用提供重要参考.

Abstract

With the rapid development of the new energy industry, lithium-ion batteries (LIBs) have been extensively applied in various fields, such as electric vehicles and energy storage devices. However, constrained by lagging recycling modes, the global annual output of spent LIBs exceeds one million tons. Spent LIBs contain scarce metals, such as cobalt, nickel, and lithium, as well as toxic components, including electrolytes and binders. The improper disposal of spent batteries is prone to resource waste and pollution of soil and water bodies. Therefore, the efficient recycling and reusing of spent LIBs have become a strategic priority for safeguarding resource security and promoting the achievement of the “dual carbon” goals. As a new type of green solvent developed by mixing hydrogen-bond donors and acceptors in a specific ratio, deep eutectic solvents (DESs) have gradually replaced traditional toxic and volatile solvents. Endowed with prominent advantages such as excellent environmental compatibility, strong recyclability, tunable physicochemical properties, and outstanding dissolution capacity for cathode metal oxides, DESs have demonstrated significant practical value and economic feasibility for the recycling of spent LIBs. This study systematically reviews the research status of spent LIBs recycling using DESs in recent years, focusing on the extraction mechanisms and core principles of valuable metals from battery cathode materials. It analyzes the separation principles of different DESs systems and clarifies the differences in their core leaching mechanisms. When exploring DES-based recycling technologies, the separation efficiency and leaching mechanism of each system are closely related to its composition and structure. For example, hydrogen bond-based DESs mainly rely on hydrogen bond interactions to promote the dissolution of metal oxides, whereas metal-based DESs may enhance the leaching efficiency through synergistic effects between metal ions and target metals. Clarifying these differences in mechanisms can provide a theoretical basis for targeted design and optimization of DESs systems. On this basis, this study further discusses the bottleneck problems faced by current DESs recycling technologies. Although DESs have shown great potential in laboratory research, many challenges remain in their practical application. For instance, the preparation cost of some high-performance DESs is relatively high, which reduces their large-scale application, and the viscosity of some DESs is too high at room temperature, which affects the mass-transfer efficiency of the leaching process and reduces the overall recycling efficiency. The separation and purification technology for the target metals in DESs leaching solutions must be further improved to realize the efficient recovery of valuable metals. Finally, this paper outlines the future technical pathways for the efficient, green, and sustainable recycling of spent LIBs using DESs. Future research should focus on the development of low-cost DESs systems, explore the use of cheap raw materials, such as biomass derivatives, to reduce preparation costs, and optimize the composition ratio of DESs to adjust their physicochemical properties and improve their leaching performance. At the same time, it is necessary to strengthen research on multi-metal synergistic separation technology to realize the selective recovery of various valuable metals in spent LIBs. This review is expected to provide important references for subsequent research and engineering applications in the field of spent LIBs recycling, and contribute to the sustainable development of the new energy industry.

关键词

低共熔溶剂 / 废旧锂离子电池 / 回收技术 / 金属浸出 / 资源循环

Key words

deep eutectic solvents / spent lithium-ion batteries / recycling technology / metal leaching / resource recycling

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基金资助

天津市杰出青年基金资助项目(25JCJQJC00320)