Chemistry evolution of LiNi1/3Co1/3Mn1/3O2-NaHSO4·H2O system during roasting

Zhang, Xiaodong; Wang, Dahui; Chen, Huaijing; Yang, Lu; Yu, Yueshan; Li, Xu

doi:10.1016/j.ssi.2019.05.018

Cited by 29 publications

(12 citation statements)

References 38 publications

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“…In this case, we can learn from the recovery of valuable metals by sulfate roasting of ternary materials (LiNi x Co y Mn 1−x−y O 2 ). 22 In the sulfate roasting method, the nickel, cobalt, and manganese elements in the ternary material (LiNi 1/3 Co 1/3 Mn 1/3 O 2 ) can be transformed from oxides to low-valence sulfates (NiSO 4 , CoSO 4 , and MnSO 4 ). Besides, Fe, Cu, and Al metals can be transformed into its corresponding sulfate (FeSO 4 , CuSO 4 , and Al 2 (SO 4 ) 3 ).…”

Section: ■ Introductionmentioning

confidence: 99%

“…From the traditional perspective, oxidative leaching shall be performed to remove elemental impurities, followed by reductive leaching to remove high-valence impurities. In this case, we can learn from the recovery of valuable metals by sulfate roasting of ternary materials (LiNi x Co y Mn 1– x – y O 2 ) . In the sulfate roasting method, the nickel, cobalt, and manganese elements in the ternary material (LiNi 1/3 Co 1/3 Mn 1/3 O 2 ) can be transformed from oxides to low-valence sulfates (NiSO 4 , CoSO 4 , and MnSO 4 ).…”

Section: Introductionmentioning

confidence: 99%

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

Gao

Wang

Zhang

et al. 2020

ACS Sustainable Chem. Eng.

146

109

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Recycling graphite from spent lithium-ion batteries plays a significant role in relieving the shortage of graphite resources and environmental protection. In this study, a novel method was proposed to regenerate spent graphite (SG) via a combined sulfuric acid curing, leaching, and calcination process. First, we conducted a sulfuric acid curing–acid leaching experiment and systematically investigated the effects of various operation conditions on the removal of impurities. Regenerated graphite was obtained after a sequential calcination at 1500 °C, and its morphology and structure were characterized by using X-ray diffraction, Raman spectroscopy, and spherical aberration electron microscopy analysis. The results show that the impurity removal efficiency by sulfuric acid curing–acid leaching is much higher than that by direct acid leaching, and the purity of the regenerated graphite can reach 99.6%. Additionally, the regenerated graphite displays favorable characteristics in morphology and structure, which are close to that of a commercial unused material. The regenerated graphite exhibits good electrochemical performance in charge capacity and cycle. The initial charge capacity and retention rate are 349 mA h/g and 98.8%, respectively. This recycle method has the advantages of low energy consumption and low waste acid discharge and can be performed by easily available equipment, so it may have great prospect for the industrial-scale recycling of SG.

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Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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

Gao

Wang

Zhang

et al. 2020

ACS Sustainable Chem. Eng.

146

109

View full text Add to dashboard Cite

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“…Zheng et al have revealed that the Ni-rich surrounding can facilitate the formation of oxygen vacancy at low temperature, which would allow the Ni ions to diffuse into the Li slab. However, a number of works have reported the delayed detection of mass loss or oxygen evolution (Figure a) because it costs time for oxygen to diffuse from the inner surface to the surface of the particle. − As illustrated in Figure , it can reasonably infer that thermal annealing promoted lattice ordering would prevail at the low-temperature (≤400 °C) region, according to the Arrhenius relationship, and higher temperature would enable more efficient reorganization of atoms in this low-temperature region. However, the structure decomposition is initiated by significant bond breaking occurred when the annealing temperature is greater than 415 °C, where formation of oxygen vacancies would allow the Ni ions to diffuse into the Li slab.…”

Section: Resultsmentioning

confidence: 99%

Tuning the Li/Ni Disorder of the NMC811 Cathode by Thermally Driven Competition between Lattice Ordering and Structure Decomposition

et al. 2020

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Ni-rich layered LiNi x Mn y Co z O2 (NMC) cathodes for lithium-ion batteries are receiving a lot of attention owing to their promising large capacity, whereas the high content of Ni results in several issues including poor thermal stability and serious Li/Ni disorder. Although a little degree of the Li/Ni disorder may be beneficial for the structural stability of NMC cathodes and even migration of Li ions, a high degree of the Li/Ni disorder certainly deteriorates their electrochemical performances. Therefore, tuning the Li/Ni disorder is of great interest in the development of safer NMC cathodes with larger accessible capacity. Post-synthesis annealing is a facile and low-cost way to manipulate lattice defects, yet has not been utilized to optimize the Ni-rich NMC cathodes. In this work, we report that post-synthesis annealing can induce the competition between lattice ordering and structure decomposition. The thermal annealing promoted that lattice ordering would prevail until the decomposition of oxygen lattice. Once the annealing temperature reaches the critical temperature to form oxygen vacancies, Ni ions can easily migrate into the Li slab. The Li/Ni disorder can be facilely tuned through post-synthesis annealing to optimize the electrochemical performances of NMC cathodes.

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“…Because of the relatively lower economic value of Li (compared with Co), it is usually recycled at the last step of the process, resulting in its overall low recovery efficiency. With the wide application of LIBs, the nonrenewable and scarce nature of Li resources makes it increasingly important to recycle Li. , However, the selective Li-extraction process currently developed has problems such as exhaust gas emission and complicated metal ion separation. − Our recent work on the recovery of LiCoO 2 (LCO) by using a conventional sulfation roasting process has demonstrated that efficient selective recovery of Li from the spent cathode materials can be achieved by controlling the content of CoSO 4 produced at room temperature without sulfur-containing waste gas emissions . Compared to the previous approaches for cathode recycling, our new strategy represents a greener LiCoO 2 cathode recovery method with higher efficiency and lower energy costs.…”

Section: Introductionmentioning

confidence: 99%

Conversion Mechanisms of Selective Extraction of Lithium from Spent Lithium-Ion Batteries by Sulfation Roasting

Lin

Fan

et al. 2020

ACS Appl. Mater. Interfaces

Self Cite

157

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With the undergoing unprecedented development of lithium-ion batteries (LIBs), the recycling of end-of-life batteries has become an urgent task considering the demand for critical materials, environmental pollution, and ecological impacts. Selective recovery of targeted element(s) is becoming a topical field that enables metal recycling in a short path with highly improved material efficiencies. This research demonstrates a process of selective recovery of spent Ni–Co–Mn (NCM)-based lithium-ion battery by systematically understanding the conversion mechanisms and controlling the sulfur behavior during a modified-sulfation roasting. As a result, Li from complex cathode components can be selectively extracted with high efficiency by only using water. Notably, the sulfur driven recovery processes can be divided into two stages: (i) part of the structure of NCM523 was destroyed, and Ni, Co, and Mn were reduced to divalent in different degrees to form sulfate (NiSO4, CoSO4, MnSO4) when reacting with H2SO4 at ambient temperature; (ii) with increasing temperature, Li ions in the unstable layered structure are released and combined with SO4 2– in the transition metal sulfate to form Li2SO4, and the sulfates of transition metals react to form Ni0.5Co0.2Mn0.3O1.4. Studies have shown sulfur can be recirculated thoroughly in the form of SO4 2–, which in principle avoids secondary pollutions. By controlling the appropriate conversion temperature, we envisage that the sulfation selective roasting recovery technology could be easily applied to other spent lithium-ion battery materials. Besides, this work may also provide a unique platform for further study on the efficient extracting of other mineral resources.

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Chemistry evolution of LiNi1/3Co1/3Mn1/3O2-NaHSO4·H2O system during roasting

Cited by 29 publications

References 38 publications

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

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

Tuning the Li/Ni Disorder of the NMC811 Cathode by Thermally Driven Competition between Lattice Ordering and Structure Decomposition

Conversion Mechanisms of Selective Extraction of Lithium from Spent Lithium-Ion Batteries by Sulfation Roasting

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