A sustainable strategy for spent Li-ion battery regeneration: microwave-hydrothermal relithiation complemented with anode-revived graphene to construct a LiFePO<sub>4</sub>/MWrGO cathode material

Jiang, Zhenyu; Sun, Jing; Jia, Pingshan; Wang, Wenlong; Song, Zhanlong; Zhao, Xinbing; Mao, Yanpeng

doi:10.1039/d1se01750k

Cited by 23 publications

(9 citation statements)

References 37 publications

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“…The regenerated cathode shows a cyclic retention of about 92 % at C/3 after 60 cycles. Jiang et al [61] demonstrated the successful relithiation of spent LiFePO 4 (LFP) batteries via the microwavehydrothermal process. They have developed a new cathode material by refurbishing the spent cathode and microwavereduced graphene oxide (MWrGO) anode for high electrochemical performances.…”

Section: Hydrothermal Process Of Relithiationmentioning

confidence: 99%

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Raj

Sahoo

Nikoloski

et al. 2022

Batteries & Supercaps

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Batteries & Supercaps www.batteries-supercaps.org Review doi.org/10.1002/batt.202200418The inherent advancement of lithium-ion batteries (LIBs) in electronic gadgets is expanding exponentially, and the ongoing surge of electric vehicles (EVS) in the near future will result in an unprecedented amount of lithium waste. Used cathode materials contain hazardous metal toxic, polymer binder, and electrolytes, posing a serious risk to the environment and public health. For socio-environmental reasons, it is required to recover all valuable metals or to immediately relithiate the used cathode materials by adding suitable salts in the stoichiometric ratio. As the consumption of batteries increases over time in daily life, recycling LIBs will become more and more crucial. Compared to the traditional hydrometallurgical and pyrometallurgical routes, direct recycling technologies can regenerate electrodes without using an intensive energy or chemicals, which saves money and reduces secondary waste. As a result, the authors emphasise direct relithiation methods for spent cathode relithiation, such as hydrothermal, ionothermal, electrochemical, and molten salts. In-depth analysis and discussion are also given to the aforementioned approaches. The deactivation, disintegration, and separation processes used in the physical processing of black mass and other constituents are discussed. We reviewed the obstacles, possible commercialization of technology, and recommendations to the reviewer for the developing ecologically friendly recycling technology in the near future toward the circular economy.

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Section: Hydrothermal Process Of Relithiationmentioning

confidence: 99%

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Raj

Sahoo

Nikoloski

et al. 2022

Batteries & Supercaps

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“…The use of mild acids coupled with microwave‐assisted heating/ultrasonication promises an environment friendly and time‐saving leaching process. [ 16–18 ]…”

Section: Introductionmentioning

confidence: 99%

“…The use of mild acids coupled with microwave-assisted heating/ultrasonication promises an environment friendly and timesaving leaching process. [16][17][18] Most battery recycling papers focus on strategies to recover elements from the parent compound. [19][20][21][22][23] For instance, Zou et al [24] employed a technology to dispose of the mixed raw cathode materials and obtained regenerated cathode materials as products with good electric performance.…”

Section: Introductionmentioning

confidence: 99%

Upcycling of Spent LiCoO₂ Cathode to Lithium Dual‐Ion Battery Anode

Suriyakumar

Pattavathi

Jojo

et al. 2023

Advanced Sustainable Systems

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Owing to the paradigm shift of the automobile industry toward the electrification of vehicles, the aftermath of batteries that power these devices at the end of their lives has to be addressed strenuously. Since upcycling strategies are hardly in the limelight, this paper focuses on giving a second life to LiCoO 2 cathode as a dual-ion battery (DIB) anode. Among many possible recovery approaches explored for cobalt, a microwave-assisted green leaching method comprising mild leaching agents is chosen for this work. Cobalt is recovered as cobalt oxalate and converted to cobalt/cobalt oxide nanospheres embedded in a porous graphitic carbon matrix (Co 3 O 4 /Co@C). Due to the high working voltage, excellent safety, and environmental friendliness, DIBs are being considered as a replacement for lithium-ion batteries in specific sectors. In an unconventional approach, the derived Co 3 O 4 /Co@C is effectively employed as an anode material for dual-ion batteries. The half-cell demonstrates a high discharge capacity of 550 mAh g −1 at 0.1 A g −1 . A full-cell DIB fabricated using Co 3 O 4 /Co@C, derived from upcycled LiCoO 2 as an anode and graphite as a cathode, shows an appreciable capacity and remarkable cycling stability. This sustainable approach for upcycling exhausted LIBs can pave the way to improve the circular economy of batteries.

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“…However, due to insufficient contact between the Li source and the spent LFP, the structure of the regenerated LFP is likely to be heterogeneous. [13,14] Hydrothermal treatment can overcome the shortcomings of the solid-state calcination method. Chen et al repaired spent LFP by hydrothermal methods with citric acid as a reducing agent followed by an annealing process.…”

Section: Introductionmentioning

confidence: 99%

“…[16] Yet, the problems regarding toxicity and the cost of reducing agents remain to be solved. [14,17,18] Another issue associated with the regenerated LFP is poor cycling stability, [13,[19][20][21][22] which hinders its practical applications. This problem occurs because LFP can provide only a 1D Li + transport channel during cycling (sluggish Li + diffusion capability), and the extracted Li + cannot return to their original Li + sites at a high current density, which induces the formation of FePO 4 (FP) phase during cycling, leaving a large number of Li + vacancies (Li V ) in the LFP.…”

Section: Introductionmentioning

confidence: 99%

Long‐Life Regenerated LiFePO₄ from Spent Cathode by Elevating the d‐Band Center of Fe

et al. 2022

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A large amount of spent LiFePO4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li+ diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li+ migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d‐band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen‐doped carbon. The FeO bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d‐band center. The Li+ diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.

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A sustainable strategy for spent Li-ion battery regeneration: microwave-hydrothermal relithiation complemented with anode-revived graphene to construct a LiFePO₄/MWrGO cathode material

Abstract: Spent LiFePO4 (LFP) cathodes were revived through a microwave-hydrothermal relithiation process, complemented with microwave-reduced graphene oxide (MWrGO) derived from spent graphite anodes, to form a composite LFP/MWrGO cathode material.

Cited by 23 publications

References 37 publications

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Upcycling of Spent LiCoO₂ Cathode to Lithium Dual‐Ion Battery Anode

Long‐Life Regenerated LiFePO₄ from Spent Cathode by Elevating the d‐Band Center of Fe

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A sustainable strategy for spent Li-ion battery regeneration: microwave-hydrothermal relithiation complemented with anode-revived graphene to construct a LiFePO4/MWrGO cathode material

Abstract: Spent LiFePO4 (LFP) cathodes were revived through a microwave-hydrothermal relithiation process, complemented with microwave-reduced graphene oxide (MWrGO) derived from spent graphite anodes, to form a composite LFP/MWrGO cathode material.

Cited by 23 publications

References 37 publications

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Retrieving Spent Cathodes from Lithium‐Ion Batteries through Flourishing Technologies

Upcycling of Spent LiCoO2 Cathode to Lithium Dual‐Ion Battery Anode

Long‐Life Regenerated LiFePO4 from Spent Cathode by Elevating the d‐Band Center of Fe

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Product

Resources

About

A sustainable strategy for spent Li-ion battery regeneration: microwave-hydrothermal relithiation complemented with anode-revived graphene to construct a LiFePO₄/MWrGO cathode material

Upcycling of Spent LiCoO₂ Cathode to Lithium Dual‐Ion Battery Anode

Long‐Life Regenerated LiFePO₄ from Spent Cathode by Elevating the d‐Band Center of Fe