Lu Zhiyong, Ning Liangmin, Zhu Xiangnan, Yu Hao
College of Energy and Mining Engineering, Shandong University of Science and Technology, Qingdao 266590, China.
College of Energy Storage Technology, Shandong University of Science and Technology, Qingdao 266590, China.
Materials (Basel). 2025 Jun 24;18(13):2987. doi: 10.3390/ma18132987.
In the wake of global energy transition and the "dual-carbon" goal, the rapid growth of electric vehicles has posed challenges for large-scale lithium-ion battery decommissioning. Retired batteries exhibit dual attributes of strategic resources (cobalt/lithium concentrations several times higher than natural ores) and environmental risks (heavy metal pollution, electrolyte toxicity). This paper systematically reviews pyrometallurgical and hydrometallurgical recovery technologies, identifying bottlenecks: high energy/lithium loss in pyrometallurgy, and corrosion/cost/solvent regeneration issues in hydrometallurgy. To address these, an integrated recycling process is proposed: low-temperature physical separation (liquid nitrogen embrittlement grinding + froth flotation) for cathode-anode separation, mild roasting to convert lithium into water-soluble compounds for efficient metal oxide separation, stepwise alkaline precipitation for high-purity lithium salts, and co-precipitation synthesis of spherical hydroxide precursors followed by segmented sintering to regenerate LiNiCoMnO cathodes with morphology/electrochemical performance comparable to virgin materials. This low-temperature, precision-controlled methodology effectively addresses the energy-intensive, pollutive, and inefficient limitations inherent in conventional recycling processes. By offering an engineered solution for sustainable large-scale recycling and high-value regeneration of spent ternary lithium ion batteries (LIBs), this approach proves pivotal in advancing circular economy development within the renewable energy sector.
在全球能源转型和“双碳”目标的背景下，电动汽车的快速增长给大规模锂离子电池退役带来了挑战。退役电池具有战略资源（钴/锂浓度比天然矿石高几倍）和环境风险（重金属污染、电解液毒性）的双重属性。本文系统综述了火法冶金和湿法冶金回收技术，找出了瓶颈问题：火法冶金中能量/锂损失高，湿法冶金中存在腐蚀/成本/溶剂再生问题。为解决这些问题，提出了一种综合回收工艺：采用低温物理分离（液氮脆化研磨+泡沫浮选）进行正负极分离，进行温和焙烧将锂转化为水溶性化合物以实现高效金属氧化物分离，采用分步碱性沉淀法制备高纯度锂盐，并通过共沉淀合成球形氢氧化物前驱体，随后进行分段烧结以再生LiNiCoMnO正极，其形态和电化学性能与原始材料相当。这种低温、精确控制的方法有效解决了传统回收工艺中固有的能源密集、污染和低效的局限性。通过为废旧三元锂离子电池（LIB）的可持续大规模回收和高价值再生提供一种工程解决方案，该方法对于推动可再生能源领域的循环经济发展至关重要。
