Characterization of Aged Li-Ion Battery Components for Direct Recycling Process Design

Fink, Kae; Santhanagopalan, Shriram; Hartig, Julia; Cao, Lei

doi:10.1149/2.0781915jes

Cited by 16 publications

(9 citation statements)

References 44 publications

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“…At both cycle 10 and cycle 50, voltage plateaus are evident for the aged material, most notably for the Ac-W-R, DEC-W-R, and IPA-W-R samples. This profile shape indicates the presence of the spinel phase and has previously been reported for this commercial material . Structural analysis will be taken up in greater detail in the subsequent section.…”

Section: Results and Discussionsupporting

confidence: 75%

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Impacts of Solvent Washing on the Electrochemical Remediation of Commercial End-Of-Life Cathodes

Fink

Gasper

Coyle

et al. 2020

ACS Appl. Energy Mater.

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Changes to the surface structure and chemistry occurring throughout the functional lifetime of lithium-ion batteries (LIBs) may impact the effectiveness of end-of-life rejuvenation methods. Solvent washing prior to electrochemical relithiation is shown to both increase relithiation efficacy and beneficially alter the interfacial chemistry of a heavily degraded industrial cathode material. Four common solvents (acetone, diethyl carbonate, isopropyl alcohol, and propylene carbonate) are employed to investigate the role of varying physicochemical solvent properties on the mechanism of capacity recovery. Electrochemical (dQ/dV, EIS), structural (XRD), and chemical (SPME-GC-MS) analysis techniques are employed to comprehensively analyze solvent–cathode interactions. Highly nucleophilic solvents (acetone, DEC) are found to reduce cathode charge-transfer impedance and enable stable impedance growth throughout subsequent cycling. The use of nucleophilic solvents under mechanically aggressive washing conditions may also enable the reintroduction of bulk lattice oxygen, thereby restoring anionic redox capacity. Further, the four solvents are found to selectively remove a subset of surface species from the aged cathode material, including residual electrolyte, additives, and electrolyte–additive reaction products, which are qualitatively analyzed. Surface species removal by each solvent is correlated with the electrochemical performance of the correspondingly washed cathode, highlighting the importance of an optimized washing protocol for effective remediation in the context of direct LIB recycling. For the material under study, the use of a simple acetone-washing protocol prior to electrochemical relithiation enables up to 174% capacity recovery relative to unwashed/relithiated black mass.

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Section: Results and Discussionsupporting

confidence: 75%

“…This profile shape indicates the presence of the spinel phase 27 and has previously been reported for this commercial material. 28 Structural analysis will be taken up in greater detail in the subsequent section.…”

Section: Resultsmentioning

confidence: 99%

Impacts of Solvent Washing on the Electrochemical Remediation of Commercial End-Of-Life Cathodes

Fink

Gasper

Coyle

et al. 2020

ACS Appl. Energy Mater.

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“…These incumbent indirect recycling methods smelt or dissolve EOL batteries and break down the cathode materials into low-value elemental constituents, which lead to high processing cost and water contamination . In contrast, the direct recycling process, just as its name implies, retrieves the high-value EOL cathode materials, retains their virgin structure and morphology, and restores the defects of electrode materials directly without chemical decompostion, indicating a small circle of a closed loop with minimal energy and environmental impact . It can be observed in Figure that the direct recycling process in the green line greatly shortens the recycling route by physical separation of components and targeted reconditioning of deficient electrodes.…”

Section: Advancements Of Direct Recyclingmentioning

confidence: 99%

“…28 In contrast, the direct recycling process, just as its name implies, retrieves the high-value EOL cathode materials, retains their virgin structure and morphology, and restores the defects of electrode materials directly without chemical decompostion, indicating a small circle of a closed loop with minimal energy and environmental impact. 29 It can be observed in Figure 1 that the direct recycling process in the green line greatly shortens the recycling route by physical separation of components and targeted reconditioning of deficient electrodes. It is capable of simplifying the regeneration process and avoiding secondary pollution, leading to an ecofriendlier and smarter recycling strategy.…”

Section: Advancements Of Direct Recyclingmentioning

confidence: 99%

Sustainable Recycling of Electrode Materials in Spent Li-Ion Batteries through Direct Regeneration Processes

Peng

Zhang

2022

ACS EST Eng.

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The prevalence of electric vehicles (EVs) globally could generate a huge number of spent Li-ion batteries (LIBs) as they reach their end of life. It is expected that by 2030, 11 million metric tons of EOL LIBs will be generated cumulatively, with annual waste flows of EV batteries reaching 34,000 t by 2040. Recycling spent LIBs in a sustainable and effective manner is a matter of utmost importance. Conventional recycling strategies such as pyrometallurgy and hydrometallurgy decompose the crystal structures of value-added electrode materials to element levels, presenting fatal drawbacks in high greenhouse gas emissions, cost, and energy consumption. The burgeoning direct recycling processes provide viable options to rejuvenate LIB compounds without chemical change, thus retaining their original composition as well as the embedded energy. Relithiation and defect restoration are the critical steps for electrode regeneration, which determine the performance of recovered material. Here, the authors provide a detailed discussion and analysis on different regeneration methods for LIB electrodes based on their degradation mechanisms. The advancements of direct recycling among other recycling technologies are highlighted through discussions of its process benefits. Physical pretreatments including deactivation, disassembly, and black mass separation are introduced. Perspectives toward scaled applications of direct recycling are also demonstrated on the basis of developing trends of future LIBs.

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“…Further publications prove that, beside these mostly investigated influences, degradation effects of electrical aging, also leading to a capacity fade of LIBs [28], must be considered in the safety assessment. These can affect the cells' TR behavior [29] and mechanical properties [18,22,[30][31][32][33]. In addition, some literature is available with respect to the influence of aging on safety.…”

Section: Introductionmentioning

confidence: 99%

Multiscale Analysis and Safety Assessment of Fresh and Electrical Aged Lithium-Ion Pouch Cells Focusing on Mechanical Behavior

et al. 2022

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Analyzing the impact of electrical aging on the lithium-ion cell’s mechanical behavior and safety is an important factor to assess the crash safety of electric vehicles during their lifetime. In this study, fresh and electrical aged state-of-the-art NCM pouch cells were investigated. Aged cells, which were cycled electrically to 90% state of health, under laboratory conditions in electric vehicle battery modules were used. The used charging/discharging strategy represents real customer behavior based on accelerated driving profiles. First, it is shown that electrical aging has a significant influence on the anodes’ and separators’ mechanical properties, which had a lower mechanical strength and stiffness under tension. Additionally, quasi-static cylindrical indentation and three-point bending tests were performed to investigate aging effects on cell level at varying state of charge (SOC). Aged cells with 0% SOC showed a right-shifted force–displacement curve and a 29% lower maximum force compared to fresh cells. Fully charged, aged cells reached a similar maximum force to fresh cells, but faster temperature increase and higher temperature peaks after internal short circuit. Inductively coupled plasma optical emission spectrometry analyses confirmed an increased lithium content on the anode surface, which is indicated in literature as a reason for the increased exothermic reaction of the aged cells. The results indicate a higher safety risk for the aged investigated pouch cells under mechanical loads based on their changed mechanical properties and thermal runaway behavior.

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Characterization of Aged Li-Ion Battery Components for Direct Recycling Process Design

Cited by 16 publications

References 44 publications

Impacts of Solvent Washing on the Electrochemical Remediation of Commercial End-Of-Life Cathodes

Impacts of Solvent Washing on the Electrochemical Remediation of Commercial End-Of-Life Cathodes

Sustainable Recycling of Electrode Materials in Spent Li-Ion Batteries through Direct Regeneration Processes

Multiscale Analysis and Safety Assessment of Fresh and Electrical Aged Lithium-Ion Pouch Cells Focusing on Mechanical Behavior

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