The rapid growth in demand for lithium‐ion batteries (LIBs) is posing challenges in the management of end‐of‐life (EoL) systems and the supply of critical raw materials (CRMs), especially lithium, cobalt, and nickel. Such challenges can be addressed by collecting and recycling spent LIBs through economically and environmentally sustainable processes and by enabling the transition to a circular economy vision based on the use of secondary raw materials. These processes involve not only the metallurgic approaches to recover the critical metals, but also the pretreatment approaches that are crucial to enhance the recovery efficiency of other valuable materials (e.g., graphite, fluorinated compounds, binders, electrolyte). Herein, pretreatment processes ranging from the disassembling, opening, and sorting to the component separation, collection, and recovery, are described for the EoL 18650‐type commercial LIB. A closed loop of eco‐friendly recycling to fully recover the composite cathode, i.e., the cathode active material (CAM), the fluorinated binder, and the conductive carbon, as well as the separator, is presented. The recovery approach is based on green solvents and is designed to limit water consumption. The recovered materials are used to assemble a new cell, and the electrochemical characterization is used to evaluate the effective feasibility of the whole recycling process.

The penetration of Li-ion batteries (LIBs) in the automotive market makes a zero-waste vision for battery recycling urgent. This can play a crucial role in developing a circular economy through the recovery of critical raw materials (CRMs) as well as bringing non-metallic components back to use. In recent years, recycling technologies for LIBs entered a new stage focused on the development of advanced pre-treatment processes to separate all the valuable battery components and more sustainable metallurgical approaches. Compared to common recycling processes, supercritical fluid (SCF) technology has great advantages related to its environmental benignity; chiefly, if CO₂ is used as the SCF (scCO₂), it is an outstanding solvent for green chemistry approaches. This review aims at providing an overview on the current progresses and open challenges of SCF technology for the treatment of end-of-life LIBs. The fundamentals of SCF technology process are discussed, providing the reader a brief overview of principles, operation procedures and instrumentation. Thereafter, the main applications in the field of battery recycling are reviewed. Successful methods for battery electrolyte recovery via scCO₂ are discussed together with pioneering studies on the extraction of critical metals from the cathode that demonstrate promising recovery rates (>60%) for Li, Co, Mn, and Ni. Finally, a specific focus is given on the huge innovation potential of scCO₂ to separate and reuse the fluorinated binder from the electrode. At present, the binder is burnt in common recycling processes, leading to hazardous fluorinated gas emissions. This review aims to emphasize the opportunities of the SCF technology in battery waste treatment as a promising approach for resource recovery with significant economy and environmental perspectives.

The Li-ion batteries (LIBs) penetration in the automotive market makes more urgent the boosting of zero-waste battery recycling. This can play a crucial role in developing a circular economy through the recovery of critical raw materials (CRMs), as well as non-metallic components back to use. In recent years, the recycling technologies for LIBs entered in a new stage focused on the development of i) advanced pre-treatment processes to separate all the valuable battery components, and ii) more sustainable metallurgical approaches. Compared to the common recycling processes, Supercritical Fluid (SCF) technology is environmentally benign, chiefly if CO2 is used as the SCF (scCO2). This review aims at providing an overview on the current progresses and the open challenges of SCF technology for the treatment of End-of-Life LIBs. The fundamentals of SCF technology process are discussed, providing the reader a brief overview of principles, operation procedures and instrumentation. Thereafter, the main applications in the field of batteries recycling are reviewed, including electrolyte recovery and high-rate extraction of critical metals from the cathode. Finally, a focus is given on the huge innovation potential of scCO2 to separate and reuse the fluorinated binder from the electrode. At present, the binder is burnt in the common recycling processes, leading to hazardous fluorinated gas emissions.

The increasing demand for Lithium-ion batteries (LIBs) in several applications, from consumer electronics to electric vehicles (EVs), has led to a substantial rise in their production, posing serious risks in the supply of critical raw materials (CRMs, e.g.: Li, Ni, Co, and graphite). Additionally, an improper disposal of end-of-life (EoL) batteries can lead to environmental pollution and loss of technological value (e.g., burning of electrolyte and fluorinated binder) stressing the necessity for a sustainable recycling. Current methods involve shredding whole batteries into a black mass, from which the components are separated through pyrometallurgy (energy-intensive) or hydrometallurgy with inorganic acids (potentially harmful to environment and workers). However, a more refined approach to LIBs recycling involves the dismantling and the sorting of their components, allowing for a targeted extraction. Here, a recycling process for spent cathodes is presented, involving the delamination from the current collector and the leaching of the cathode active material (CAM) into the same citric acid (CA) solution; this also enables the recovery of PVDF and Carbon conducting filler as a residue of the leaching. Lastly, the metals recovered as precursors, are used to resynthesize fresh CAM, thus closing the recycling loop.