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[Display omitted] • ·Offer guidance for the application and improvement of LIB recycling technologies. • ·Quantitatively compare LIB recycling technologies in terms of environment and economy. • ·Emphasize the importance of priority recycling Li to the future LIB recovery. • ·Identify two directions for the future development of firstly recycling Li technology. • ·Unravel the technical essence and underlying challenges for LIB recycling. The recycling of lithium-ion battery (LIB) is becoming a global concern due to its vast quantity, underlying danger, and supply crisis of critical metals. Despite the recent development of various LIB recycling technologies, it remains unclear whether these technologies are suitable for large-scale application. This perspective aims to review and evaluate the application potential of these emerging technologies and seeks to channel the true laboratory innovations into the industry. We redefine and categorize the emerging technologies with a focus on lithium recovery, and quantitatively compare them in terms of environmental impact and economic feasibility. The advantages and urgency of prioritizing lithium recovery in LIB recycling are highlighted. Additionally, we discuss the principles of these technologies, identify the key factors, limitations, and suggestions for improvement of these emerging technologies. Finally, we explore future challenges that LIB recycling may face from the aspects of policy, market risk, and industry competition. This Perspective will contribute to more efficient, environmentally friendly, and economically viable LIB recycling efforts. [ABSTRACT FROM AUTHOR]

The large-batch application of lithium ion batteries leads to the mass production of spent batteries. So the enhancement of disposal ability of spent lithium ion batteries is becoming very urgent. This study proposes an integrated process to handle bulk spent lithium manganese (LiMn 2 O 4 ) batteries to in situ recycle high value-added products without any additives. By mechanical separation, the mixed electrode materials mainly including binder, graphite and LiMn 2 O 4 are firstly obtained from spent batteries. Then, the reaction characteristics for the oxygen-free roasting of mixed electrode materials are analyzed. And the results show that mixed electrode materials can be in situ converted into manganese oxide (MnO) and lithium carbonate (Li 2 CO 3 ) at 1073 K for 45 min. In this process, the binder is evaporated and decomposed into gaseous products which can be collected to avoid disposal cost. Finally, 91.30% of Li resource as Li 2 CO 3 is leached from roasted powders by water and then high value-added Li 2 CO 3 crystals are further gained by evaporating the filter liquid. The filter residues are burned in air to remove the graphite and the final residues as manganous-manganic oxide (Mn 3 O 4 ) is obtained. [ABSTRACT FROM AUTHOR]

Spent lithium-ion batteries (LIBs) have been one of the fast-growing and largest quantities of solid waste in the world. Spent graphite anode, accounting for 12–21 wt% of batteries, contains metals, binders, toxic, and flammable electrolytes. The efficient recovery of spent graphite is urgently needed for environmental protection and resource sustainability. Recently, more and more studies have been focused on spent graphite recycling, while the advance and challenges are rarely summarized. Hence, this study made a comprehensive review of graphite recycling including separation, regeneration, and synthesis of functional materials. Firstly, the pretreatment of graphite separation was overviewed. Then, the spent graphite regeneration methods such as leaching, pyrometallurgy, their integration processes, etc. were systematically introduced. Furthermore, the modification strategies to enhance the electrochemical performance were discussed. Subsequently, we reviewed in detail the synthesis of functional materials using spent graphite for energy and environmental applications including graphene, adsorbents, catalysts, capacitors, and graphite/polymer composites. Meanwhile, we briefly compared the economic and environmental benefits of graphite regeneration and other functional materials production. Finally, the technical bottlenecks and challenges for spent graphite recycling were summarized and some future research directions were proposed. This review contributes to spent LIBs recycling more efficiently and profitably in the future. [Display omitted] • The pretreatment of spent graphite separation is overviewed. • The regeneration methods and enhanced performance of spent graphite are summarized. • The synthesis of functional materials using spent graphite is emphasized. • The technical bottlenecks and challenges in spent graphite recycling are discussed. [ABSTRACT FROM AUTHOR]

The rapid development of new energy technology leads to explosive growth of lithium-ion batteries (LIBs) industry which greatly alleviates the problems of environmental pollution and energy shortage. However, how to realize resource circulation of critical metals including lithium (Li) and cobalt (Co) becomes the new problem of LIBs industry. This paper proposes an improved thermal reduction technology to efficiently recycle Li and Co from spent LIBs, where cheap urea is applied as the only additive to provide ammonia (NH 3). By thermal reduction, LiCoO 2 was thermally reduced into water-soluble lithium carbonate and water-insoluble cobalt metal Under the optimal conditions, 99.96% Li with nearly 100% selectivity was obtained by water leaching. More importantly, the concept of "oxygen elements removal (OER)" was proposed to explain the metal extraction from spent LIBs, which could help to describe the reaction mechanism as O-cage digestion mechanism. Furthermore, metal extraction from spent LIBs was re-understood as "seeking an applicable reductant", which provided a fresh perspective for understanding Li selective recovery. These concepts and findings can provide some inspiration for metal recovery from spent LIBs. [Display omitted] • Cheap urea as the only additive is used for thermal reduction of LiCoO 2. • The optimal 99.96% Li leaching rate with nearly 100% selectivity is obtained. • The Concept of "oxygen elements removal" is proposed to explain metal extraction. • Different LIBs chemistries are processed by this way to realize Li selective recovery. [ABSTRACT FROM AUTHOR]

Spent lithium-ion batteries (LIBs) recycling has attracted much attention because it is highly favorable to environment protection and sustainable development. Developing a cleaner method for metals extraction can greatly reduce risk of secondary pollution. Chlorinating technology has been proved as an efficient method for metals extraction instead of traditional hydrometallurgy. In this paper, cathode materials from spent LIBs could be rapidly converted into metal chlorides by NH 4 Cl roasting at 623 K for 20 min. The results indicated nearly 100% metal leaching rates were achieved. Further, in-depth study is performed to obtain the mechanism function of chlorinating conversion based on roasting and TGA experiments. The apparent activation energy as 73.40 kJ/mol was firstly obtained, and then the reaction model of chlorination reaction was determined by model fitting and verifying. Herein, sub-reactions of chlorination reaction were figured out and their contributions were used to determinate reaction controlling mechanisms of chlorination reaction. The results indicated that nucleation reaction played a leading role in the initial stage (0.05 < α < 0.43) while phase boundary reaction took the control in next stage (0.43 < α < 0.95), which gave a good explanation to activation energy change. Finally, our findings provided inspirations for studying the controlling mechanism of gas-solid reaction. ga1 • Nearly 100% metal leaching rates are achieved by chlorinating conversion. • Contribution of sub-reactions is used to determinate reaction controlling mechanism. • The reaction controlling mechanism is determined to explain activity energy change. [ABSTRACT FROM AUTHOR]

A targeted extraction technology for recycling lithium from spent lithium transition metal oxides (LTMO) type batteries is developed in this paper. The chlorinating technology with ammonium chloride as the only additive is employed and controlled to selectively extract lithium. High lithium extraction rate with a low selectivity was first obtained at non-controlled chlorinating conditions. During this process, it was found that the reducing driving force (RDF) played a vital role in metals extraction. Once RDF was controlled at a low level, lithium elements could be targetedly extracted out while other metal elements still remained in the residues. The results showed that 91.73% lithium elements were leached out with a selectivity of 90.04% at the optimal conditions. Further, the mechanism was proposed to explain the release behavior of metals from cathode materials from the perspective of extracting driving force. These principles also offer inspiration for metal selective extraction fields such as metallurgy and recovery of complex systems including multiple metals. ga1 • Chlorination conversion is controlled to realized the targeted extraction of lithium. • Metal release behavior is studied from the perspective of extracting driving force. • High Li recovery and selectivity rate is gained by controlled chlorination technology. [ABSTRACT FROM AUTHOR]

Wet leaching has been commonly applied to separate metals out from spent lithium ion batteries (LIBs), and large volumes of chemicals including acids and additives are required to reach high metal separation efficiencies. To reduce heavy use of chemicals for metal separation becomes significant in cleaner production. We propose a dry-phase process as chlorination conversion for separating metals from spent LIBs with low-stoichiometric amounts of additive. With ammonium chloride (NH 4 Cl) as the only additive, high metal separating efficiencies are achieved. Based on theoretical analysis and experimental investigation, it was found that chlorination conversion was promoted in a relatively closed environment and the suitable reaction temperature was between 623 K and 800 K. By parameter optimization, nearly 100% extracting efficiencies of Li and Co were achieved at 673 K for 20 min with the mass ratio of w(LiCoO 2)/w(NH 4 Cl) as 1:2 under air atmosphere. Furthermore, the reaction mechanism was described as a two-step process which could be illustrated as the dry-extraction of LiCoO 2. Finally, an acid-free approach was developed to realize the efficient metal extraction from cathode materials of spent LIBs. Image 1 • An acid-free process for metal separation from spent lithium ion battery is proposed. • High metal separating efficiency is obtained with NH 4 Cl as the only additive. • A dry-extraction mechanism is proposed to explain the metal separation. [ABSTRACT FROM AUTHOR]

Recycling valuable metals from the batteries has aroused much attention recently. However, the elimination of residual electricity is often neglected, and NaCl-discharging is commonly used to release residual electricity from spent LIBs without consideration of the environmental impacts. In this paper, experimental studies are carried out in different solutions to investigate the discharge efficiency and environmental impacts. The results show that the discharge rate is much slow only by water electrolysis, and the discharge rate can be greatly improved with the participation of solution ions in the discharge process. Besides, the high discharge efficiency always results in high risks of environment pollution. MnSO 4 solution with a mild discharge rate is proved as a choice to reduce galvanic corrosion and avoid organic leakage. Therein, the isolation layer was in-situ formed to avoid oxygen corrosion. Finally, the O 2 -control mechanism is proposed to explain the cleaner process of battery discharge in MnSO 4 solution. Image 1 • Battery discharge in salt solution is more than a simple short-circuit process. • High discharge efficiency always results in high risks of environment pollution. • An in-situ protection way is applied to mildly and environmentally discharge battery. • The O 2 -control mechanism is proposed to explain the battery discharge process. [ABSTRACT FROM AUTHOR]