Data underlying the publication: A Closer Look at Lithium-Ion Batteries in E-waste and the Potential for a Universal Hydrometallurgical Recycling Process

Abstract<br>The demand for lithium-ion batteries (LiBs) is rising, resulting in a growing need to recycle the critical raw materials (CRMs) which they contain. Typically, all spent LiBs from consumer electronics end up in a single waste stream that is processed to produce black mass (BM) for further recovery. It is desired to design a recycling process that can deal with a mixture of LiBs. Hence, this study investigates the structure and composition of battery modules in common appliances such as laptops, power banks, smart watches, wireless earphones and mobile phones. The battery cells in the module were disassembled into cell casing, cathode, anode and separator. Then, the cathode active materials (CAMs) were characterized in detail with XRD-, SEM-, EDX- and ICP-OES-analysis. No direct link was found between the chemistry of the active materials (NMC, LCO, LMO, LFP etc.) and the application. Various BM samples were submitted to a leaching procedure (2 M H₂SO₄, 50 °C, 2 hr, 60 g BM/L) with varying concentration (0-4 vol%) of H₂O₂to study the influence of their chemical composition on the dissolution of Li, Ni, Mn and Co. Only a part of the BMs dissolved completely at 4 vol% H₂O₂, which was attributed to the oxidation state of the transition metals (TMs). Exact determination of H₂O₂ consumption by redox titration confirmed this hypothesis.

摘要：锂离子电池（Lithium-ion Batteries, LiBs）的需求持续增长，使得其所含关键原材料（critical raw materials, CRMs）的回收需求日益迫切。当前，消费电子领域产生的所有废弃锂离子电池均汇入单一废物流，经处理后得到黑渣（black mass, BM）以用于后续有价金属回收。为设计可适配混合锂离子电池的回收工艺，本研究针对笔记本电脑、移动电源、智能手表、无线耳机及手机等常见消费电子产品的电池模块结构与组成展开探究。研究人员先将模块内的电芯拆解为电芯外壳、正极、负极与隔膜，随后采用X射线衍射（XRD）、扫描电子显微镜（SEM）、能量色散X射线光谱（EDX）及电感耦合等离子体发射光谱仪（ICP-OES）等手段对正极活性材料（cathode active materials, CAMs）进行详细表征。研究未发现活性材料的化学体系（如镍钴锰三元材料（NMC）、钴酸锂（LCO）、锰酸锂（LMO）、磷酸铁锂（LFP）等）与电池应用场景之间存在直接关联。本研究选取多组黑渣（BM）样品，采用浓度范围为0~4%（体积分数）的过氧化氢（H₂O₂）与2 mol/L硫酸（H₂SO₄）组成的浸出体系，在50℃、固液比60 g BM/L的条件下反应2小时，探究黑渣化学组成对锂、镍、锰、钴溶出行为的影响。仅部分黑渣样品在过氧化氢浓度为4%（体积分数）时实现完全溶解，该现象归因于过渡金属（transition metals, TMs）的氧化价态差异。通过氧化还原滴定法精准测定过氧化氢消耗量，验证了上述假说。