Effective separation of LiNi0.5Co0.2Mn0.3O2cathode material and Al foilviadigestion of PVDF enabling a closed-loop recycle

Qin, Zuoyu; Li, Jiaqi; Zhang, Tao; Wen, Zuxin; Zheng, Zhicheng; Zhang, Ying; Zhang, Ning; Jia, Chuankun; Liu, Xiaohe; Chen, Gen

doi:10.1039/d2ta06959h

Cited by 16 publications

(4 citation statements)

References 48 publications

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“…Obviously, the R ct in R-NCM523 is almost half of the S-NCM523, even slight smaller than commercial NCM523 (denoted as C-NCM523), indicating the fluent Li + channel of the regenerated particles, which may result from the well recovery of the layered structure. [23] As expected, R-NCM523 delivers the 90.3% retention of initial specific capacity (143.7 mA h g −1 ) after 200 cycles (Figure S7g, Supporting Information), higher than C-NCM523 of 78.5% capacity retention (145.9 mA h g −1 for initial capacity). Also, the superior ability of R-NCM523 for storing capacity still can be reflected by high current rate test (from 3 to 5 C in Figure S7f, Supporting Information).…”

Section: Resultssupporting

confidence: 73%

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode

Qin,

Zhang,

Gao

et al. 2023

Advanced Materials

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The ever‐growing demand for resources sustainability has promoted the recycle of spent lithium‐ion batteries (LIBs) to a strategic position. Direct recycle outperforms either hydrometallurgical or pyrometallurgical approaches due to the high added value and facile treatment processes. However, the traditional direct recycling technologies are only applicable for Ni‐poor/middle cathodes. Herein, we directly recycle of spent Ni‐rich LiNi0.8Co0.1Mn0.1O2 (S‐NCM) to performance‐enhanced single‐crystalline cathode materials using a simple but effective LiOH‐NaCl molten salt. We systematically investigate the evolution process of the Li‐supplement and grain‐recrystallization during regeneration, and comprehensively prove the successful recovery of the highly degraded microstructure, including significant elimination of Ni2+ and O vacancies. Beneficial from the favorable reconstructed single‐crystalline particles, the regenerated NCM (R‐NCM) represents remarkably enhanced structural stability, electrochemical activity, O2 and cracks suppression during charge/discharge, thus achieving the excellent performances in long‐term cycling and high‐rate tests. As a result, R‐NCM maintains the 86.5% reversible capacity at 1C after 200 cycles. Instructively, the present molten salt can be successfully applied for recycling spent NCMs with various Li and Ni compositions (e.g., LiNi0.5Co0.2Mn0.3O2).This article is protected by copyright. All rights reserved

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Section: Resultssupporting

confidence: 73%

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode

Qin,

Zhang,

Gao

et al. 2023

Advanced Materials

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“…Even after 250 cycles, the curves of R‐NCA are nearly identical as the first one; while the profile in C‐NCA becomes oblique and voltage platform disappears in Figure S7, demonstrating the severe capacity fading and electrochemical polarization of C‐NCA. Figure 6e exhibits the results of internal resistance measurement with the equivalent circuit model inserted within the picture, in which the R ct (diameter of the semicircle in the Nyquist plot) stands for the charge transfer resistance [7d, 27] . It is noteworthy that the parameter of R ct in C‐NCA is almost three times than that in R‐NCA.…”

Section: Resultsmentioning

confidence: 99%

A Universal Molten Salt Method for Direct Upcycling of Spent Ni‐rich Cathode towards Single‐crystalline Li‐rich Cathode

et al. 2023

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With ever‐increasing pursuit for high‐value output in recycling spent lithium‐ion batteries (LIBs), traditional recycling methods of cathodes tend to be obsolete because of the complicated procedures. Herein, we first upcycle spent polycrystal LiNi0.88Co0.095Al0.025O2 (S‐NCA) to high value‐added single‐crystalline and Li‐rich cathode materials through a simple but feasible LiOH‐Na2SO4 eutectic molten salt strategy. The in situ X‐ray diffraction technique and a series of paratactic experiments record the evolution process of upcycling and prove that excessive Li occupies the transition metal (TM) layers. Beneficial from the single‐crystalline and Li‐rich nature, the regenerated NCA (R‐NCA) exhibits remarkably enhanced electrochemical performances in terms of long‐term cyclability, high‐rate performance and low polarization. This approach can also be successfully extended to other cathode materials e.g., LiNixCoyMnzO2 (NCM) and mixed spent NCAs with varied degree of Li loss.

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“…As far as we know, although numerous efforts have been devoted to the direct regeneration of LCO, NMC, − and LFP − cathode materials, very few works are reported in the literature dealing with the direct reconditioning of NCA CAMs. Specifically, LiNi 0.8 Co 0.15 Al 0.05 O 2 is one of the most successful compositions of the NCA-based cathode materials.…”

Section: Introductionmentioning

confidence: 99%

Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

Oubaha,

Fkhar,

Cloots

et al. 2024

ACS Sustainable Resour. Manage.

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The steadily growing lithium-ion batteries (LIBs) market brings the critical question of the future treatment of tremendous waste from end-of-life (EoL) LIBs. Therefore, recycling of EoL LIBs has become an urgent need to overcome the foreseen environmental and economic challenges. Herein, we propose a direct recycling process to regenerate NCA cathode active material (CAM) from spent LIBs. A gentle heat pretreatment at a low temperature is applied to facilitate the recovery of the CAMs. The cathode strips from EoL LIBs were subjected to two temperatures (150 or 250 °C) during a short time (2 h) to deactivate the strong bonding between the polyvinylidene difluoride binder and the Al current collector surface. Thus, the CAM is easily and fully reclaimed from the Al foil. Moreover, the developed procedure preserves the integrity of the NCA structure without any morphological changes. The full restoration of NCAbased CAM powder is successfully achieved through Li-replenishing using Li 2 CO 3 under O 2 atmosphere at different sintering temperatures (750 or 900 °C). The healed NCA CAMs demonstrate decent electrochemical performance including good cyclability and rate performance in NCA//Li half-cell and NCA//LTO full-cell configurations.

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Effective separation of LiNi_0.5Co_0.2Mn_0.3O₂cathode material and Al foilviadigestion of PVDF enabling a closed-loop recycle

Abstract: With ever-growing market of electric vehicles, the spent lithium-ion batteries (LIBs) eventually turn into a huge challenging issue to both environment and resource sustainability. Recycling the valuable components in spent...

Cited by 16 publications

References 48 publications

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode

A Universal Molten Salt Method for Direct Upcycling of Spent Ni‐rich Cathode towards Single‐crystalline Li‐rich Cathode

Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

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Effective separation of LiNi0.5Co0.2Mn0.3O2cathode material and Al foilviadigestion of PVDF enabling a closed-loop recycle

Abstract: With ever-growing market of electric vehicles, the spent lithium-ion batteries (LIBs) eventually turn into a huge challenging issue to both environment and resource sustainability. Recycling the valuable components in spent...

Cited by 16 publications

References 48 publications

Self‐Reconstruction of Highly Degraded LiNi0.8Co0.1Mn0.1O2 toward Stable Single‐Crystalline Cathode

Self‐Reconstruction of Highly Degraded LiNi0.8Co0.1Mn0.1O2 toward Stable Single‐Crystalline Cathode

A Universal Molten Salt Method for Direct Upcycling of Spent Ni‐rich Cathode towards Single‐crystalline Li‐rich Cathode

Direct NCA Cathode Active Materials Recycling from Spent Li-Ion Batteries: Solvent-Free Recovery and Healing by Heat Treatment

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Product

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Effective separation of LiNi_0.5Co_0.2Mn_0.3O₂cathode material and Al foilviadigestion of PVDF enabling a closed-loop recycle

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode

Self‐Reconstruction of Highly Degraded LiNi_0.8Co_0.1Mn_0.1O₂ toward Stable Single‐Crystalline Cathode