Ternary cathodes account for more than half of the Lithium-Ion Batteries (LIBs) cathode market share and their recycling draws the most attention. Solvent extraction is the most efficient and common method to separate and recover Co and Ni from spent ternary cathode leachates. However, the traditional extraction process produces a large amount of saline wastewater, thus will seriously pollute the environment. In this work, an environmental approach is proposed by adding a water-soluble complexing agent into the aqueous phase, the separation factor is 2 times higher and the consumption of NaOH is 90% reduced compared to the Na-saponified counterpart, which was attributed to the differences of the complexation between metal ions and complexing agent in aqueous phase. The differences in the complexing ability are enhanced with an increased local nucleophilicity index of the active sites along with a reduced molecular volume in complexing agent, thus leading to superior cobalt extraction efficiency (∼98.9%) and separation factor (∼345). In addition, because of the fact that the whole-process pollution control is needed for cleaner chemical production, a green process is developed by recovering additives through Tri-n-butyphosphate. This excellent separation performance suggests that adding complexing agent in solvometallurgical recovery process may aid in the future development of high-purity raw metals for advanced fields.

三元正极占锂离子电池（LIBs）正极市场份额的一半以上，其回收利用最受关注。溶剂萃取是从废三元阴极浸出液中分离和回收钴和镍的最有效和最常用的方法。然而，传统的提取工艺会产生大量含盐废水，严重污染环境。在这项工作中，提出了一种环保方法，即在水相中添加水溶性络合剂，与钠皂化的对应物相比，分离因子提高了 2 倍，NaOH 的消耗量减少了 90%，这归因于金属离子与络合剂在水相中络合的差异。络合能力的差异随着活性位点的局部亲核性指数的增加以及络合剂中分子体积的减小而增强，从而导致优异的钴提取效率（~98.9%）和分离因子（~345）。此外，由于清洁化工生产需要全程污染控制，因此开发了通过磷酸三正丁回收添加剂的绿色工艺。这种优异的分离性能表明，在溶剂冶金回收过程中添加络合剂可能有助于未来高纯度金属原料的先进领域开发。此外，由于清洁化工生产需要全程污染控制，因此开发了通过磷酸三正丁回收添加剂的绿色工艺。这种优异的分离性能表明，在溶剂冶金回收过程中添加络合剂可能有助于未来高纯度金属原料的先进领域开发。此外，由于清洁化工生产需要全程污染控制，因此开发了通过磷酸三正丁回收添加剂的绿色工艺。这种优异的分离性能表明，在溶剂冶金回收过程中添加络合剂可能有助于未来高纯度金属原料的先进领域开发。