High reversibility of layered oxide cathode enabled by direct Re-generation

Guo, Yaqing; Liao, Xiaobin; Huang, Pengjie; Lou, Ping; Su, Yaqiong; Hong, Xufeng; Han, Qigao; Yu, Ruohan; Cao, Yuan‐Cheng; Chen, Shijie

doi:10.1016/j.ensm.2021.09.016

Cited by 64 publications

(44 citation statements)

References 36 publications

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“…At present, the research subject of the direct regeneration method is the NCM micron secondary particles formed by the agglomeration of nanometer primary particles. , The random crystal orientation of primary particles produces significant stress due to volume change during cycling, which promotes grain boundary cracking among primary particles. , The exposed cracks lead to continuous penetration of the electrolyte, which gradually extends from the surface of the secondary particles to the primary particles. The formation of new reaction interfaces means that degradation of the surface structure is extended.…”

Section: Introductionmentioning

confidence: 99%

Single-Crystal Materials Regenerated and Modified by Spent NCM523 as a High-Voltage Stable Cycling Cathode Material

Dong

Wang

et al. 2022

ACS Sustainable Chem. Eng.

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In recent years, the direct regeneration of cathode materials has attracted the attention of a large number of researchers because of its advantages of a simple process and high metal utilization rate. The grain boundary cracking of secondary agglomeration particles will aggravate the degradation of batteries during cycling. In this work, we propose the idea of regenerating spent NCM523 from secondary agglomeration particles into micron single crystals. This approach combines mechanical activation and high-temperature annealing. The regenerated single-crystal materials not only recover the layered structure but also have the same electrochemical reaction kinetics as the single-crystal materials synthesized by the precursors. In addition, a simple and practical solution is proposed, in which LiAlO2 is coated on the surface of the material by hydrolysis and high-temperature annealing. The capacity retention rate of the 1 mol % LiAlO2-coated single-crystal material is 97.49% after 100 cycles of 0.2 C charge/1 C discharge cycling at 3.0–4.5 V. The high Li ionic conductivity of LiAlO2 reduces the charge transfer impedance of single-crystal particles at high voltage and alleviates surface side reactions, achieving cycling stability. This new method provides a feasible scheme for sustainable utilization of cathode materials.

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Section: Introductionmentioning

confidence: 99%

Single-Crystal Materials Regenerated and Modified by Spent NCM523 as a High-Voltage Stable Cycling Cathode Material

Dong

Wang

et al. 2022

ACS Sustainable Chem. Eng.

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“…A full-battery (1.7 Ah) test demonstrated that the renovated NCM523 cathode materials showed an exceptional cycling performance of 500 cycles with high capacity retention of 90.8%. [45] To examine the regeneration mechanism of cathode materials by the hydrothermal approach, Xu et al systematically studied the effects of experimental parameters on microstructures, compositions, and electrochemical performances of the renovated cathode materials. [145] It can be seen from the contour map that, compared with the hydrothermal temperature factor, the relithiation time was observed to be more important for obtaining high-performance regenerated cathode materials (Figure 8d).…”

Section: Hydrothermal Methodsmentioning

confidence: 99%

“…A full‐battery (1.7 Ah) test demonstrated that the renovated NCM523 cathode materials showed an exceptional cycling performance of 500 cycles with high capacity retention of 90.8%. [ 45 ]…”

Section: Regeneration Strategiesmentioning

confidence: 99%

“…Generally, the LIBs retire when losing more than 20% of the initial capacity, yet, the bulk structure of electrode materials remains largely intact. [45,46] Decades of studies have revealed that, after the long-term cycles, the capacity degradation of each cathode material can be mainly ascribed to Li loss, phase transformation, surface reconstruction, TM dissolution, and particle cracking, which highly depends on the service conditions of different cathode materials. [47][48][49][50][51] As shown in Figure 3a, Zheng and co-workers conducted a deep cycling experiment on commercial 18650 LiFePO 4 /graphite battery with 1900 cycles and disclosed that the Li loss is the major cause for capacity degradation.…”

Section: Introductionmentioning

confidence: 99%

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Advances in Intelligent Regeneration of Cathode Materials for Sustainable Lithium‐Ion Batteries

Jin

Zhang

2022

Advanced Energy Materials

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policies in clean energy industry. [10][11][12] As shown in Figure 1a, it is conservatively estimated that the shipment volume of LIBs in 2025 (439.32 GWh) is nearly doubled compared with that in 2021 (237.44 GWh) and the corresponding global market closes to $106.81 billion, mainly resulting from the great popularization of electric vehicles. In addition, based on market analysis and forecast, the percent of LIBs with lithium iron phosphate (LFP) and lithium nickel cobalt manganese oxide (NCM) cathode materials is continuously increasing at a high speed (Figure 1b), which will firmly dominate the market for a long time because of their notably technical advantages. [13,14] There is no doubt that the mature LIBs industry really brings a great number of benefits to our life, such as the convenience and cleanliness. [15][16][17] However, as every coin has two sides, some key issues behind the popularized LIBs applications cannot be neglected. Lithium (Li) metal and other transitional metals (TMs) like cobalt (Co), nickel (Ni), and manganese (Mn) have been consumed in large quantities to manufacture the cathode materials for fulfilling the tremendous production of LIBs. [18][19][20][21] These metallic resources are rare on the earth with high cost and limited geographic distribution. Moreover, the Co and Ni metals are toxic, which are not environmental-friendly and jeopardize to human health. [11,[22][23][24] Therefore, in the back of prosperity of LIBs, we are also facing the emerging resources crisis and seriously secondary environmental pollution problems as long as the massive retired LIBs are present and not appropriately treated in following several years. [25][26][27] To make "Waste-be-Wealth," the effective strategy should be employed to tackle the waste LIBs problems in a green and sustainable way. [28,29] Nowadays, the conventional pyrometallurgical and hydrometallurgical technologies are only two existing industrial approaches in recycling the cathode materials of retired LIBs, which, yet, just focus on the recovery target of rare metallic resources (e.g., Co, Ni, and Li) from faded cathode materials. [30,31] As illustrated in Figure 2, in terms of the pyrometallurgical method, it usually involves the high temperature process to smelt the end-of-life cathode materials, in which the valuable metal elements are sintered into alloy forms after several purification and separation processes. Thus, this process usually needs high energy consumption and will unavoidably Explosively increased market penetration of lithium-ion batteries (LIBs) in electric vehicles, consumer electronics, and stationary energy storage devices has recently aroused new concerns on nonrenewable metal resources and environmental pollution because of the forthcoming wave of retired popularized LIBs. Recycling the retired LIBs in an environmentally sustainable and cost-effective way thus becomes much urgent and imperative. As a preferable route, the direct regeneration strategy has been innovatively proposed to repair degraded cathode mat...

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“…235 Based on the failure mechanism analysis of LIB cathode materials, it is found that LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) cathode materials have problems such as the dissolution of Li and transition metals, surface interface failure and structural transformation. 222,[236][237][238] Combined with the above analysis, NCM523 material can be directly regenerated by supplementing metal ions, granulation, ion doping and heat treatment (Fig. 14d).…”

Section: Other Cutting-edge Technologiesmentioning

confidence: 99%

Emerging green technologies for recovery and reuse of spent lithium-ion batteries – a review

et al. 2022

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High reversibility of layered oxide cathode enabled by direct Re-generation

Cited by 64 publications

References 36 publications

Single-Crystal Materials Regenerated and Modified by Spent NCM523 as a High-Voltage Stable Cycling Cathode Material

Single-Crystal Materials Regenerated and Modified by Spent NCM523 as a High-Voltage Stable Cycling Cathode Material

Advances in Intelligent Regeneration of Cathode Materials for Sustainable Lithium‐Ion Batteries

Emerging green technologies for recovery and reuse of spent lithium-ion batteries – a review

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