Graphite Recycling from the Spent Lithium-Ion Batteries by Sulfuric Acid Curing–Leaching Combined with High-Temperature Calcination

Gao, Yang; Wang, Chengyan; Zhang, Jialiang; Jing, Qiankun; Ma, Baozhong; Chen, Yongqiang; Zhang, Wenjuan

doi:10.1021/acssuschemeng.0c02321

Cited by 139 publications

(119 citation statements)

References 31 publications

(48 reference statements)

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“…Generally, residual cathode materials, and elemental Cu, Fe, Al, and other contaminants, can be found in the leaching residue. [181] Commonly, oxidative lixiviation using acids and other solvents can be used to remove impurities including Al, Cu, and Fe whereas reductive lixiviation can be used to remove remaining cathode metals from the recycled graphite powders. [182] Recently organic acid such as citric acid has been used to regenerate graphite from the spent anode.…”

Section: Reusability Of Graphite From Green Recycling Processmentioning

confidence: 99%

Green Recycling Methods to Treat Lithium‐Ion Batteries E‐Waste: A Circular Approach to Sustainability

et al. 2021

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E‐waste generated from end‐of‐life spent lithium‐ion batteries (LIBs) is increasing at a rapid rate owing to the increasing consumption of these batteries in portable electronics, electric vehicles, and renewable energy storage worldwide. On the one hand, landfilling and incinerating LIBs e‐waste poses environmental and safety concerns owing to their constituent materials. On the other hand, scarcity of metal resources used in manufacturing LIBs and potential value creation through the recovery of these metal resources from spent LIBs has triggered increased interest in recycling spent LIBs from e‐waste. State of the art recycling of spent LIBs involving pyrometallurgy and hydrometallurgy processes generates considerable unwanted environmental concerns. Hence, alternative innovative approaches toward the green recycling process of spent LIBs are essential to tackle large volumes of spent LIBs in an environmentally friendly way. Such evolving techniques for spent LIBs recycling based on green approaches, including bioleaching, waste for waste approach, and electrodeposition, are discussed here. Furthermore, the ways to regenerate strategic metals post leaching, efficiently reprocess extracted high‐value materials, and reuse them in applications including electrode materials for new LIBs. The concept of “circular economy” is highlighted through closed‐loop recycling of spent LIBs achieved through green‐sustainable approaches.

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Section: Reusability Of Graphite From Green Recycling Processmentioning

confidence: 99%

Green Recycling Methods to Treat Lithium‐Ion Batteries E‐Waste: A Circular Approach to Sustainability

et al. 2021

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“…Additionally, chlorine gas has been employed to convert the metals and oxides into metal chlorides at a temperature of 1000–1100 °C in which evolving Cl 2 is toxic to the environment. [ 25,26 ]…”

Section: Present Status Of Lib Recycling In Industriesmentioning

confidence: 99%

“…The regenerated graphite also exhibited an initial charge capacity of 349 mAh g −1 , and it claimed no wastewater generation in this process encourages us to find more routes to purify the graphite efficiently. [ 25 ] Also, it is noteworthy to include the reuse of graphite, if the structure gets distorted as a result of the several charge–discharge cycles. This type of damaged structure certainly can be employed as an electrode for the reversible Na‐storage process with carbonate‐based electrolytes owing more number of defects in their layered structure.…”

Section: Research Progress Of the Graphite Reuse In Lab‐scale: Energymentioning

confidence: 99%

An Urgent Call to Spent LIB Recycling: Whys and Wherefores for Graphite Recovery

Natarajan

Aravindan

2020

Advanced Energy Materials

196

120

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diffuse between their layers, though only at prismatic surfaces as well as it is also possible via defect sites for the basal planes. The term "intercalation in graphite" refers to the incorporation of atomic or molecular layers of a guest species between the ordered graphite layers, and this process would be reversible and "topotactic" that endorses the different interlayer distance without changing the carbon atomic arrangement within the layer. The mechanism involved in the intercalation process is generally identified as "staging" where the lithium prefers to reside in the distant graphene layers first rather than picking the neighbor graphene layers as shown in Figure 1; however, Li-ions pick the gap of neighboring graphene layers to form a Li-C 6-Li-C 6 chain along the c-direction if the graphite is intercalated fully with a spacing of 0.430 nm. [3,4,6-8] As well, it is also proven that both hexagonal and rhombohedral graphitic phases could able to intercalate the lithium reversibly almost in the same storage capacities. Commercial graphite possesses a larger number of rhombohedral units, and that kind of graphene planes as a host will be more favorable to intercalate lithium. Many efforts have been made to clarify the intercalation mechanism of lithium into the graphite from various perspectives. The occurrence of solid electrolyte interphase (SEI) formation is necessary for safe operation (since LiC 6 is known to be the strong reducing agent) of the cell regardless of any electrode/electrolyte contact and plays a decisive role in the capacity of the material. [9] It is well-known that the excess charge consumption for the graphite-based electrodes during the first cycle surpasses the theoretical capacity of 372 mAh g-1 as a result of this passive layer formation, i.e., SEI, also attributed to the corrosion-like reactions of Li x C 6. The intercalated compounds are unstable similar to metallic lithium in the electrolytes which surface is protected by this formation of SEI layer that pays the excess charge consumption in the first cycle of the intercalation/deintercalation process. Generally, non-graphitic carbons which have not c-direction in the crystallographic order can be categorized as high (x > 1 in Li x C 6) and low (x = 0.5-0.8 in Li x C 6) specific charge carbons based on their reversible lithium storage properties. From the category of low-specific charge carbons, coke and turbostratic kind of carbons gain much attention for the Li-intercalation owing to their structural properties, which could overwhelm the development of Li x (solv) y C 6. Also, the coke-containing electrode unveiled the reversible Li-intercalation at ≈1.2 V versus Li during the first cycle, distinguishes from the insertion potential of graphite because of the disordered structure. High specific Spent lithium-ion batteries (LIBs) are a key source for securing tons of raw materials that are valuable materials for LIB applications. However, the massive emerging volume of spent LIBs urgently needs a new management strategy to recy...

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“…Spent graphite is first harvested from spent LIBs using physical separation methods similar to those in pyrometallurgy or hydrometallurgy before thermal pretreatment steps to eliminate organic impurities and binders, allowing them to be exfoliated from the current collectors [21]. Subsequently, acid leaching (e.g., with H 2 SO 4 ) is conducted to extract imbedded Li as well as other metal impurities [32]. The extracted Li is then precipitated using NaOH/Na 2 CO 3 to produce Li 2 CO 3 , a precursor for new battery material synthesis.…”

Section: Anode Recyclingmentioning

confidence: 99%

Emerging trends in sustainable battery chemistries

Tan

Chen

2021

Trends in Chemistry

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Graphite Recycling from the Spent Lithium-Ion Batteries by Sulfuric Acid Curing–Leaching Combined with High-Temperature Calcination

Cited by 139 publications

References 31 publications

Green Recycling Methods to Treat Lithium‐Ion Batteries E‐Waste: A Circular Approach to Sustainability

Green Recycling Methods to Treat Lithium‐Ion Batteries E‐Waste: A Circular Approach to Sustainability

An Urgent Call to Spent LIB Recycling: Whys and Wherefores for Graphite Recovery

Emerging trends in sustainable battery chemistries

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