Ligand-driven cooperative leaching of spent battery cathodes

Massive spent lithium-ion batteries will peak soon, creating energy, environment, economy, and technology challenges and key metal supply burdens in all resource-relevant industries. Here, we develop a universal energy-effective, sustainable, and easily modularized recycling strategy to retrieve transition metals and lithium from spent cathodes (LiCoO2 and LiNi0.8Co0.1Mn0.1O2) via a high-capacity cooperative leaching process. The high-capacity leaching with acid-free sustainable agents is enabled by strong coordination using green deep eutectic solvents and synergistic strong ligand molecules through a concurrent reduction-dissolution and direct coordination mechanism. Importantly, the Al foil current collector, binder, and carbon additives remain non-dissolved under our mild treatment condition and can be easily filtered out, which is vastly more advantageous than conventional hydro/pyrometallurgy processes that involve complicated purification. Furthermore, as a demonstration of high-value applications, we transform the leached solution to high-quality single or ternary atomic catalysts and LiCl, completing the loop for recycling spent battery cathodes.