The recycling of spent lithium-ion batteries (Li-ion Batteries) has drawn a lot of interest in recent years in response to the rising demand for the corresponding high-value metals and materials and the mounting concern emanating from the detrimental environmental effects imposed by the conventional disposal of solid battery waste. Numerous studies have been conducted on the topic of recycling used Li-ion batteries to produce either battery materials or specific chemical, metal or metal-based compounds. Physical pre-treatment is typically used to separate waste materials into various streams, facilitating the effective recovery of components in subsequent processing. In order to further prepare the recovered materials or compounds by applying the principles of materials chemistry and engineering, a metallurgical process is then utilized to extract and isolate pure metals or separate contaminants from a particular waste stream. In this review, the current state of spent Li-ion battery recycling is outlined, reviewed, and analyzed in the context of the entire recycling process, with a particular emphasis on hydrometallurgy; however, electrometallurgy and pyrometallurgy are also comprehensively reviewed. In addition to the comprehensive review of various hydrometallurgical processes, including alkaline leaching, acidic leaching, solvent (liquid-liquid) extraction, and chemical precipitation, a critical analysis of the current obstacles to process optimization during Li-ion battery recycling is also conducted. Moreover, the energy-intensive nature of discussed recycling process routes is also assessed and addressed. This study is anticipated to offer recommendations for enhancing wasted Li-ion battery recycling, and the field can be further explored for commercialization.

The strong adhesion between cathode materials and aluminium (Al) foil substrates presents a significant challenge in the recycling of spent lithium-ion batteries (LiBs). Conventionally, high temperatures and high concentrations of costly organic solvents such as N-methyl-2-pyrrolidone (NMP), dimethylacetamide (DMAC), dimethylformamide (DMF), and dimethyl sulfoxide (DMSO) are used to enhance ultrasonication-based delamination. In this study, a novel, eco-efficient approach was demonstrated for delaminating cathode materials from Al foil using a low-concentration organic citric-acid-assisted low-power ultrasonic treatment coupled with a gentle, low-power-per-volume mechanical mixing system at room temperature. The separation mechanism was attributed to the structure disruption, possibly swelling, of the polyvinylidene fluoride (PVDF) binder using low-concentration citric acid and the cavitation effects induced by ultrasound. Key parameters influencing the delamination efficiency included the solvent type, temperature, ultrasonic power, and treatment duration. Under optimised conditions, citric acid was used as the sonication reagent, with a process temperature of 20 °C, 60 W ultrasonic power, and 80 min of ultrasonication; a delamination efficiency of approximately 92% was achieved. The recovered cathode materials exhibited low agglomeration, favouring subsequent leaching processes. This work proposes an environmentally friendly and effective method for cathode and Al foil recovery from spent LiBs, integrating manual dismantling, ultrasonic treatment, and material separation.