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Lithium-ion batteries (LIBs) are widely used in the mobile electronics, power, energy storage and other fields due to their excellent electrochemical performance, but their limited service life has resulted in a large number of spent LIBs being discarded. Due to the advantages of high recovery efficiency and mild reaction conditions, the combined pyro-hydrometallurgical process for recovering valuable metal elements from spent LIBs is emerging in line with the principles of green chemistry and has potential for large-scale industrial applications. Here we review current developments in the combined recovery process, aiming to figure out the challenges and future directions for the combined process. In detail, thermal pretreatment methods for collecting the cathode material from spent LIBs, the combined recovery process for treating the cathode material, and the subsequent separation and extraction process are summarized. Furthermore, the practical application of combined recycling schemes is demonstrated. Finally, the development and challenges of the combined process in recycling spent LIBs are revealed. Achieving pollution-free emissions and high-value utilization of spent LIB resources with low-cost treatment are future directions for the combined process. [ABSTRACT FROM AUTHOR]

As the economy recovered from the COVID-19 epidemic, the price of Li 2 CO 3 skyrocketed to the highest. Recovery of lithium from spent lithium-ion batteries (LIBs) is significant for addressing lithium shortage and environmental issues. Sulfation roasting is often accused of being unsustainable and not environmentally friendly due to the consumption of expensive sulfation reagents and emission of SO 2. Herein, a novel and green recycling process for selective separation of lithium from spent LiMn 2 O 4 (LMO) batteries was proposed based on a SO 2 emission free sulfation roasting with waste copperas. Lithium in the cathode power were selectively sulfated into soluble Li 2 SO 4 with a conversion of 99.50%, while manganese was riched as insoluble oxides. At low temperature (e.g. 400 °C), LMO were difficult to be sulfated due to the limited sulfation ability of SO 4 2- and mass transfer. When the roasting temperature reached 700 °C, SO 2 was produced and the generated SO 2 reacted in situ with the LMO to form Li 2 SO 4 and MnSO 4 , preventing SO 2 emissions into the atmosphere. As temperature continued to increase, the MnSO 4 acted as a sulfation reagent and sulfated the unreacted LMO. All the sulfur was immigrated in Li 2 SO 4 , rather than being emitted as SO 2. [Display omitted] [ABSTRACT FROM AUTHOR]