Advanced Energy Materials
·
2024
·Vol. 14
·期 26
·2401197
·
IF 24.4
Mingli Xu,Chen Wu,Lang Ye,Yuanteng Zhang,Chenyi Zhang,Jieming Hu,Ran Tan,Dong Gu,Xuanze Wang,Olivier Fontaine,Chun Zhan,Lin Zhuang,Xinping Ai,Jiangfeng Qian
Degraded LiCoO 2 cathode from retired Li-ion batteries is urgently required to be recycled in a greener way for economic and environmental considerations. The coarse metallurgy technologies for Li/Co extraction with massive CO 2 emission and energy consumption cannot satisfy the requirements of carbon neutralization. Herein, it is proposed that direct regeneration of degraded LiCoO 2 cathode could be realized via 9-fluorenone-mediated Li supplementation and follow-up structural restoration. The 9-fluorenone-lithium reagent is elaborately selected to compensate for the missing Li + into lattice with targeted stoichiometry owing to its compatible redox potential of 1.95 V versus Li + /Li, which is located just between the reversible intercalation (3.8 V) and irreversible conversion (1.2 V) potentials of LiCoO 2 electrode. Then, thermal energy-driven structure reorganization enables Li/Co atoms to occupy the right sites, accomplishing desirable structure healing within a short annealing time of 4 h. The regenerated LiCoO 2 cathode exhibits comparable Li-storage capability to commercial LiCoO 2 , benefiting from the non-destructive direct regeneration technology. In addition, the regeneration route is regarded as environmentally (0.13 kg CO 2 kg −1 cell) and economically (10.07 $ kg −1 cell) superior to conventional recycling routes based on life-cycle analysis. The precise surgery on spent LiCoO 2 cathode provides a promising solution for the forthcoming retirement rush of Li-ion batteries.
研究领域:
材料科学
·
环境科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2023
·Vol. 17
·期 3
·1163-1174
·
IF 32.5
Ganxiong Liu,Wang Wan,Quan Nie,Can Zhang,Xinlong Chen,Weihuang Lin,Xuezhe Wei,Yunhui Huang,Ju Li,Chao Wang
A persistent challenge plaguing lithium-ion batteries (LIBs) is the consumption of active lithium with the formation of SEI. This leads to an irreversible lithium loss in the initial cycle and a gradual further exhaustion of active lithium in subsequent cycles. While prelithiation has been proven effective in compensating for this loss by introducing additional active lithium into batteries, prior studies have predominantly concentrated on offsetting the initial lithium loss, often overlooking the continuous lithium consumption that occurs throughout cycling. To address this challenge, we employed a sustained in situ lithium replenishment strategy that involves the systematic release of additional lithium inventory through precise capacity control during long-term cycling. Our method utilizes a lithium replenishment separator (LRS) coated with dilithium squarate-carbon nanotube (Li2C4O4–CNT) as the lithium compensation reagent. Placing Li2C4O4 on the separator rather than within the cathode significantly reduces disruptions in conduction pathways and inhibits catalytic reactions with LiFePO4, preventing the formation of carbon residues. When implemented in the LiFePO4||graphite battery system, our approach resulted in an impressive 12.9% capacity improvement in the initial cycle and a remarkable 97.2% capacity retention over 700 cycles, surpassing the comparison group, which exhibited 80% capacity retention after 426 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chenkun Li,Yao Xiao,Xiaosong Zhang,Hongwei Cheng,Ya-Jun Cheng,Yonggao Xia
The irreversible capacity loss of lithium-ion batteries during initial cycling directly leads to a decrease in energy density, and promising lithium cathode replenishment can significantly alleviate this problem. In response to the problems of complex preparation, instability in air, and unfavorable residue of the conventional cathode lithium replenishment materials, a Li2CO3/carbon nanocomposite is prepared and utilized as the lithium replenishment material. With high-speed ball-milling, a nanocomposite with a tight embedment structured Li2CO3/Ketjen Black (KB) composite composed of nanosized Li2CO3 and KB is synthesized. The decomposition potential of Li2CO3 is effectively decreased to 3.8 V, and the amount of the active lithium ion being released is significantly increased, corresponding to a specific capacity of 645.2 mAh·g–1 during the initial charging cycle. It has been introduced into the full-cells composed of the NCM523 cathode and graphite anode, resulting in a capacity increase of 44 mAh·g–1 in the initial cycle and a 26.4% improvement in capacity retention over 100 cycles. The working mechanism of the Li2CO3/KB nanocomposite as the lithium replenishment agent has been discussed. The outcome of the work provides a practically feasible route to realize lithium-ion battery technology with improved energy density and cycling life.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Zhaofeng Zhuang,Junfeng Li,Haocheng Ji,Zhihong Piao,Xinru Wu,Guanjun Ji,Song Liu,Jun Ma,Di Tang,Nengzhan Zheng,Junxiong Wang,Guangmin Zhou
The direct recycling of cathode materials in lithium-ion batteries is important for environmental protection and resource conservation. The key regeneration processes are composition replenishment and atom rearrangement, both of which depend on the migration and diffusion of atoms. However, for the direct recycling of degraded LiNi 0.5 Co 0.2 Mn 0.3 O 2 (D-NCM523) cathode, the irreversible phase transitions that accumulate during the long-term cycles block the Li diffusion channels with a high diffusion energy barrier, making it difficult to fully repair the layered structure and resulting in rapid capacity decay. To address the challenge, fast Li replenishment channels are rebuilt to regulate the surface phase and effectively assist the regeneration process with a reduced energy barrier. This method reduces the amount of Li supplement by >75% and shortens the sintering time (only 2 h) to fully regenerate D-NCM523, compared to general direct recycling methods. The regenerated NCM523 (LCMB-NCM523) exhibits a satisfactory repaired specific capacity of 160 mAh g −1 and excellent cycling stability, retaining 78% of its capacity after 300 cycles. In addition, LCMB-NCM523 is recycled with improved thermal decomposition peak temperature and enables 200 cycles even at 60 °C, greatly improving safety. This work proposes a promising way for the large-scale direct regeneration of layered cathodes.
研究领域:
材料科学
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电池技术
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环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）