Devising an energy-efficient, profitable, and safe technology to recycle lithium-ion batteries (LIBs) is crucial for their continuous adoption in electric vehicles and grid energy storage. Herein, using recyclable electron donors (REDs) for which the redox potentials range between cathode operation and over-lithiation potentials, we establish thermodynamically controlled Li-coupled electron transfer from REDs to cathodes as a viable route for directly regenerating spent cathodes in dry air at room temperature. Simple soaking of the spent cathode in a regeneration solution enables the complete recovery of the original chemical composition and capacity of the Li-deficient cathode through electron and Li-ion transfer from RED molecules and Li salts, respectively. The RED-based lithiation universally applies to cathode materials with heterogeneous Li loss, allowing the Li quantification and cathode separation processes to be bypassed for recycling. We further demonstrate the practical feasibility of this approach by regenerating spent cathodes from commercial 1-A h pouch cells. In addition, we show that the used regeneration solution can be refreshed by simply mixing with reductants for reuse in lithiation, thereby promising minimal cost and chemical waste for battery recycling. The proposed cathode regeneration method under ambient temperature and pressure will propel the development of facile and scalable LIB recycling technologies.

中文翻译：

---

在环境条件下使用可回收电子供体对废电池阴极进行热力学控制的化学再生

设计一种节能、有利可图且安全的技术来回收锂离子电池（LIB）对于电动汽车和电网储能的持续采用至关重要。在此，使用氧化还原电位介于阴极操作和过度锂化电位之间的可回收电子供体（RED），我们建立了从RED到阴极的热力学控制的锂耦合电子转移，作为在干燥空气中直接再生废阴极的可行途径。室内温度。将废正极简单地浸泡在再生溶液中，可以通过分别从红色分子和锂盐转移电子和锂离子，完全恢复缺锂正极的原始化学成分和容量。基于RED的锂化普遍适用于具有异质Li损失的正极材料，从而可以绕过Li定量和正极分离过程进行回收。我们通过从商业 1-A h 软包电池中再生废阴极，进一步证明了这种方法的实际可行性。此外，我们还表明，通过简单地与还原剂混合即可更新用过的再生溶液，以便在锂化中重新使用，从而有望将电池回收的成本和化学废物降至最低。所提出的环境温度和压力下的阴极再生方法将推动简便且可扩展的锂离子电池回收技术的发展。