With a rapid expansion in electric vehicles, a huge amount of the spent Li-ion batteries (LIBs) could be discharged in near future. And thus, the proper handling of the spent LIBs is essential to sustainable development in the industry of electrical vehicles. Among various approaches such as pyrometallurgy, hydrometallurgy, and direct recycling, the hydrometallurgical manner has gained interest in recycling the spent LIBs due to its high effectiveness in recycling raw materials (e.g., lithium, nickel, cobalt, and manganese). However, the hydrometallurgical process not only requires the use of large amounts of acids and water resources but also produces toxic gases and wastewater leading to environmental and economic problems, considering potential economic and environmental problems. Thus, this review aims to provide an overview of conventional and state-of-the-art hydrometallurgical processes to recover valuable metals from spent LIBs. First, we briefly introduce the basic principle and materials of LIBs. Then, we briefly introduce the operations and pros-and cons- of hydrometallurgical processes. Finally, this review proposes future research directions in hydrometallurgy, and its potential opportunities in the fundamental and practical challenges regarding its deployment going forward.

This study focuses on the development of an alkaline leaching hydrometallurgy process for the recovery of tungsten from WC/Co hardmetal sludge, and an examination of the effect of the process parameters on tungsten recovery. The alkaline leaching hydrometallurgy process has four stages, i.e., oxidation of the sludge, leaching of tungsten by NaOH, refinement of the leaching solution, and precipitation of tungsten. The WC/Co hardmetal sludge oxide consists of WO3 and CoWO4. The leaching of tungsten is most affected by the leaching temperature, followed by the NaOH concentration and the leaching time. About 99% of tungsten in the WC/Co hardmetal sludge is leached at temperatures above 90oC and a NaOH concentration above 15%. For refinement of the leaching solution, pH control of the solution using HCl is more effective than the addition of Na2S·9H2O. The tungsten is precipitated as high-purity H2WO4·H2O by pH control using HCl. With decreasing pH of the solution, the tungsten recovery rate increases and then decrease. About 93% of tungsten in the WC/Co hardmetal sludge is recovered by the alkaline leaching hydrometallurgy process.