Effect of Na from the leachate of spent Li-ion batteries on the properties of resynthesized Li-ion battery cathodes

Beak, Mincheol; Park, Sanghyuk; Park, Jangho; Jeong, Seongdeock; Thirumalraj, Balamurugan; Jeong, Goojin; Kim, Taehyeon; Kwon, Kyungjung

doi:10.1016/j.jallcom.2021.159808

Cited by 34 publications

(10 citation statements)

References 50 publications

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“…Noticeably, the first semicircles in a high frequency region that are related to the film resistance induced by the formation of solid electrolyte interphase (SEI) between electrodes and electrolytes gradually shrank with an increased cycle number from 10 to 50 in both samples (see the insets in the figures). It is hard to intuitively interpret the abnormal phenomenon about the gradual decrease of film resistance, which is contrary to other relevant research [30,31]. In the meantime, the second semicircles in a low frequency region regarding charge transfer resistance (Rct) indicated incremental trends in both samples during cycling due to the structural degradation of the cathode active materials.…”

Section: Resultscontrasting

confidence: 61%

Utilizing the Intrinsic Thermal Instability of Swedenborgite Structured YBaCo4O7+δ as an Opportunity for Material Engineering in Lithium-Ion Batteries by Er and Ga Co-Doping Processes

Park

Shin

et al. 2021

Materials

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We firstly introduce Er and Ga co-doped swedenborgite-structured YBaCo4O7+δ (YBC) as a cathode-active material in lithium-ion batteries (LIBs), aiming at converting the phase instability of YBC at high temperatures into a strategic way of enhancing the structural stability of layered cathode-active materials. Our recent publication reported that Y0.8Er0.2BaCo3.2Ga0.8O7+δ (YEBCG) showed excellent phase stability compared to YBC in a fuel cell operating condition. By contrast, the feasibility of the LiCoO2 (LCO) phase, which is derived from swedenborgite-structured YBC-based materials, as a LIB cathode-active material is investigated and the effects of co-doping with the Er and Ga ions on the structural and electrochemical properties of Li-intercalated YBC are systemically studied. The intrinsic swedenborgite structure of YBC-based materials with tetrahedrally coordinated Co2+/Co3+ are partially transformed into octahedrally coordinated Co3+, resulting in the formation of an LCO layered structure with a space group of R-3m that can work as a Li-ion migration path. Li-intercalated YEBCG (Li[YEBCG]) shows effective suppression of structural phase transition during cycling, leading to the enhancement of LIB performance in Coulombic efficiency, capacity retention, and rate capability. The galvanostatic intermittent titration technique, cyclic voltammetry and electrochemical impedance spectroscopy are performed to elucidate the enhanced phase stability of Li[YEBCG].

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Section: Resultscontrasting

confidence: 61%

Utilizing the Intrinsic Thermal Instability of Swedenborgite Structured YBaCo4O7+δ as an Opportunity for Material Engineering in Lithium-Ion Batteries by Er and Ga Co-Doping Processes

Park

Shin

et al. 2021

Materials

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“…Accordingly, the trace amount of impurities that are not fully eliminated from the leachate are incorporated during the co-precipitation for the direct regeneration of cathode active materials and affect the electrochemical performance of the resynthesized cathode active materials. In our previous study, the effects of impurity elements including iron, aluminum, tin, lithium, copper, and sodium were investigated individually at impurity levels [10][11][12][13][14][15][16]. It was reported that Li[Ni 1/3 Mn 1/3 Co 1/3 ]O 2 (NMC) containing trace amounts of Fe or Al via co-precipitation showed better LIB performance in terms of cyclability and rate capability compared to a pristine sample [10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Effect of Residual Trace Amounts of Fe and Al in Li[Ni1/3Mn1/3Co1/3]O2 Cathode Active Material for the Sustainable Recycling of Lithium-Ion Batteries

et al. 2021

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As the explosive growth of the electric vehicle market leads to an increase in spent lithium-ion batteries (LIBs), the disposal of LIBs has also made headlines. In this study, we synthesized the cathode active materials Li[Ni1/3Mn1/3Co1/3]O2 (NMC) and Li[Ni1/3Mn1/3Co1/3Fe0.0005Al0.0005]O2 (NMCFA) via hydroxide co-precipitation and calcination processes, which simulate the resynthesis of NMC in leachate containing trace amounts of iron and aluminum from spent LIBs. The effects of iron and aluminum on the physicochemical and electrochemical properties were investigated and compared with NMC. Trace amounts of iron and aluminum do not affect the morphology, the formation of O3-type layered structures, or the redox peak. On the other hand, the rate capability of NMCFA shows high discharge capacities at 7 C (110 mAh g−1) and 10 C (74 mAh g−1), comparable to the values for NMC at 5 C (111 mAh g−1) and 7 C (79 mAh g−1), respectively, due to the widened interslab thickness of NMCFA which facilitates the movement of lithium ions in a 2D channel. Therefore, iron and aluminum, which are usually considered as impurities in the recycling of LIBs, could be used as doping elements for enhancing the electrochemical performance of resynthesized cathode active materials.

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“…It should be noted that sodium contamination in co-precipitation method seems to remain only on the surface of the precursor, which is different from the sodium pollution problem in spray drying. At the cost of washing with a large amount of water, the co-precipitation method can greatly eliminate sodium pollution, and even promote the residual sodium to reduce the surface film resistance of the cathode electrode and increase its lithium ion coefficient . However, the advanced anhydrous granulation technology represented by the spray drying method and sol–gel method cannot avoid the serious problem of sodium pollution.…”

Section: Resultsmentioning

confidence: 99%

Unveiling Sodium Ion Pollution in Spray-Dried Precursors and Its Implications for the Green Upcycling of Spent Lithium-Ion Batteries

Liu

Han

et al. 2021

Environ. Sci. Technol.

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Unclear impurity pollution is one of the key scientific problems that limit the large-scale production of new lithium-ion batteries (LIBs) from spent LIBs. This work is the first to report the pollution path, pollution degree, and solution method of sodium ions in the recycling process of spent LIBs in the real world. The results show that sodium ions can intrude into the precursor particles to form crystalline salts with the anion of the leaching acid that cover the transition metal elements, thereby resulting in a failed precursor. Specifically, the intrusion of sodium ions will produce a variety of pollutants containing metal oxide bonds, such as Na–O, NaO2, and Na+–O2, on the precursor surface. These active lattice oxygen will further adsorb or react to form organic oxygen, chemical oxygen, and free oxygen, which will highly deteriorate the surface cleanliness. Strictly controlling the consumption of sodium salt in each step and using ammonia instead of NaOH for pH regulation can effectively solve sodium ion pollution to prepare high-quality battery precursors. It reveals that for the green upcycling of spent LIBs, we should strengthen the design of the recycling process to reduce the consumption of chemical reagents, which will produce unexpected secondary pollution.

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Effect of Na from the leachate of spent Li-ion batteries on the properties of resynthesized Li-ion battery cathodes

Cited by 34 publications

References 50 publications

Utilizing the Intrinsic Thermal Instability of Swedenborgite Structured YBaCo4O7+δ as an Opportunity for Material Engineering in Lithium-Ion Batteries by Er and Ga Co-Doping Processes

Utilizing the Intrinsic Thermal Instability of Swedenborgite Structured YBaCo4O7+δ as an Opportunity for Material Engineering in Lithium-Ion Batteries by Er and Ga Co-Doping Processes

Effect of Residual Trace Amounts of Fe and Al in Li[Ni1/3Mn1/3Co1/3]O2 Cathode Active Material for the Sustainable Recycling of Lithium-Ion Batteries

Unveiling Sodium Ion Pollution in Spray-Dried Precursors and Its Implications for the Green Upcycling of Spent Lithium-Ion Batteries

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