CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Meiting Huang,Haoxuan Yu,Liang Chen,Haitao Yang,Zhihao Wang,Yifeng Li,Kechun Chen,Chenxi Xu,Liming Yang,Xubiao Luo
To face the large–scale retirement of lithium–ion batteries (LIBs), direct regeneration of spent NCM622 (LiNi 0.6 Co 0.2 Mn 0.2 O 2 ) cathode can effectively alleviate the current resource and environmental pressures. During the recycling process, the binder polyvinylidene fluoride (PVDF) inevitably becomes an inherent impurity in the active material. Whether the inherent impurity can assist the regeneration of spent NCM or not is becoming a focus of attentions. Hereby, a closed–loop direct regeneration strategy that transforms the inherent PVDF impurity into a F dopant is proposed, and a LiNO 3 –LiOH eutectic molten system is utilized to repair the elemental loss and structural defects in highly degraded NCM622 cathode while achieving F doping. It is found that the fluorine element is uniformly doped into both the surface and bulk phases of the whole material. The F–containing regenerated NCM cathode (R–NCM622–F) shows a stable layered structure with markedly suppressed lattice oxygen escape, as substantiated by the experimental analysis and theoretical calculation. As a result, the obtained R–NCM622–F exhibits a satisfactory repaired specific capacity of 169.6 mAh g −1 and excellent cycling stability, which retains 85.8 % of its initial capacity after 200 cycles. Meanwhile, it can deliver a considerable capacity of 120mAh g −1 even at a high rate of 5C. Clearly, our regeneration strategy obviates the necessity for intricate pretreatments, and instead employs the inherent PVDF impurity to achieve the direct regeneration process, thereby offering a promising avenue to the large–scale direct regeneration of layered cathodes.
研究领域:
材料科学
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环境科学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Meiting Huang,Zhihao Wang,Haitao Yang,Liming Yang,Kechun Chen,Haoxuan Yu,Chenxi Xu,Yingying Guo,Penghui Shao,Liang Chen,Xubiao Luo
The direct regeneration method, recognized for its cost-effectiveness, has garnered considerable attentions in the field of battery recycling. In this study, a novel direct regeneration strategy is proposed to repair spent LiFePO 4 (S-LFP) cathodes without the need for impurity removal. Instead, the residual conductive carbon and polyvinylidene fluoride (PVDF) in S-LFP are employed as inherent reductive agents. Systematic characterization and analysis reveal that the failure of S-LFP primarily originates from a substantial loss of Li + and the conversion of LiFePO 4 to FePO 4 . Meanwhile, it is demonstrated that both residual conductive carbon and PVDF play positive roles in promoting the regeneration of S-LFP through distinct mechanisms. As a result, the regenerated LFP exhibits significant recovery in crystal structure and chemical composition as compared to S-LFP, which leads to notably improved lithium storage performance. Furthermore, to further enhance the lithium storage property, a specific amount of glucose (10 %) is introduced during the regeneration of S-LFP, yielding a regenerated product that performs comparably to commercial LFP. Clearly, our approach, in contrast to traditional regeneration methods, maximizes the utilization of residual impurities within S-LFP, resulting in effective regeneration of S-LFP, thereby proving both informative and cost-effective.
研究领域:
材料科学
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能源技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Sirui Nie,Yuhao Xia,Yuzhang Xiao,Weihao Lin,Guangyao Yang,Weiliang Peng,Sikai Peng,Fanbo Meng,Renzong Hu,Bin Yuan
With the widespread adoption of lithium iron phosphate (LiFePO4, LFP)-based power batteries, it is anticipated that a huge volume of spent LFP cathodes will be generated in the near future. Therefore, it is imperative to develop advanced, ecofriendly, and efficient recycling technologies for spent LFP cathodes. In this work, a low-temperature direct hydrothermal regeneration strategy with a rapid eluting process is introduced for the spent LFP cathodes. This regeneration strategy can effectively achieve multiple goals, including supplementing Li+ ions, eliminating irreversible phase transitions, maintaining the bulk initial structure, and repairing the evenly carbon-coated layer. Moreover, the regenerated LFP can induce the formation of a thinner and more uniform CEI film during the initial charge–discharge process, achieving a fast Li+ ion diffusion rate, enhanced discharge capability, and improved structural stability. Thus, the regenerated LFP exhibits a high initial discharge capacity of 164.2 mAh g–1 at a 0.1 C rate with an initial Coulombic efficiency of 98% and 132 mAh g–1 at 5 C with a remarkable capacity retention rate of 93.1% after 800 cycles. Specifically, this direct regeneration method is shorter in process and lower in cost compared with the traditional hydrometallurgy, enabling an eco-friendly regeneration under a mild environment, which shows a huge development potential in industrial applications.
研究领域:
材料科学
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环境工程
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能源技术
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED MATERIALS
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2022
·Vol. 35
·期 5
·2208034
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IF 32.086
Kai Jia,Jun Ma,Junxiong Wang,Zheng Liang,Guanjun Ji,Zhihong Piao,Runhua Gao,Yanfei Zhu,Zhaofeng Zhuang,Guangmin Zhou,Hui-Ming Cheng
A large amount of spent LiFePO 4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li + diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li + migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d-band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen-doped carbon. The Fe O bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d-band center. The Li + diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
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2024
·Vol. 14
·期 26
·2401197
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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
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环境科学
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能源工程
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产品关联
DOI
高影响因子
RARE METALS
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2025
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IF 11
Li Xiang,Li Gui-Dong,Chen Ye,Tian Meng-Kui
Lithium iron phosphate (LiFePO 4 , LFP) batteries have shown extensive adoption in power applications in recent years for their reliable safety, high theoretical capability and low cost. Nevertheless, the finite lifespan of these batteries necessitates the future processing of a significant number of spent LFP batteries, underscoring the urgent need for the development of both efficient and eco-friendly recycling methods. This study combines the advantages of wet leaching and direct regeneration methods, leveraging citric acid’s multifaceted role to streamline the combined leaching and hydrothermal processes. Results indicate that citric acid efficiently leaches all elements from spent LFP batteries. Furthermore, through its unique structure, it enhances hydrothermal regeneration by stabilizing metal ions and controlling crystal growth, and also acts as a carbon source for the surface carbon coating of regenerated LFP (R-LFP). The R-LFP shows outstanding electrochemical stability, achieving a discharge capacity of 155.1 mAh·g −1 at 0.1C, with a capacity retention rate of 93.2% after 300 cycles at 1C. Furthermore, economic and environmental analyses demonstrate this method’s superior cost-effectiveness and sustainability. Therefore, the method proposed in this study is efficient, simple and avoids the complex process of element separation, innovatively using a single reagent to achieve closed-loop recycling of LFP batteries, providing a novel and effective solution for the resource sustainability application. Graphical abstract
研究领域:
材料科学
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环境科学
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能源工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yuyun Li,Qingfeng Liu,Wanquan Yu,Chenchen Li,Zitong Fei,Qi Meng,Peng Dong
The wide application of LiFePO 4 (LFP) batteries in energy storage equipment inevitably produces a large number of spent LFP batteries. However, the existing direct regeneration technology usually only pays attention to the compensation of Li + , ignoring the problems of poor conductivity, binder residue, and slow compensation channels of Li + in spent LFP. Here, we introduce a direct, efficient, and environmentally sustainable regeneration method of spent LFP cathodes, which utilizes argon plasma ball milling to effectively decompose the residual binder on the surface, induce the construction of vacancies in the carbon layer, and broaden the Li + compensation channels. Through argon plasma ball milling pretreatment, the Fe (III) phase can be more effectively transform into the Fe (II) phase during the calcination stage, achieving structural repair of spent LFP. The regenerated LFP exhibits excellent electrochemical performance, with the discharge capacity of 142.9 mAh g −1 at 1C, with no significant capacity loss after 200 cycles, and nearly 100 % capacity retention after 500 cycles at 5C. Economic analysis indicates that the proposed regeneration method offers significant economic benefits and low energy consumption, providing a novel reference for the efficient direct regeneration of spent lithium-ion batteries.
研究领域:
材料科学
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环境科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
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2023
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IF 20.4
Zitong Fei,Yongyou Su,Qi Meng,Peng Dong,Yingjie Zhang
Current recycling strategies for spent cathode materials mostly rely on destructive reconstruction methods to recover valuable metals; thus, sustainable improvements are urgently required to achieve the low-carbon and short-range recycling of spent lithium-ion batteries. Herein, we report a deep eutectic solvent consisting of ethylene glycol lithium, betaine, and urea (BEU) for the direct regeneration of spent LiCoO 2 materials under 80 °C and normal pressure conditions. From an initial capacity of 208.87 mAh/g, the regenerated material achieved a capacity retention rate of 87.10% after 200 cycles. The BEU method achieves direct regeneration of spent LiCoO 2 materials through restoring the lack of original composition and defects in the lattice structure. As such, it provides a new platform for the use of a variety of spent lithium cathode resources.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Meng Xiao,Xiaopeng Fu,Meihua Chen,Meng Ye,Chaoqiong Zhu,Fang Wan,Xiaodong Guo
With the massive application of lithium-ion batteries in electric vehicles, spent lithium iron phosphate (LFP) batteries have accumulated in recent years, inducing an urgent requirement in recycling technology. Direct repair technology has been considered as a promising approach for recycling spent LFP. However, the traditional solid-phase repair technology is limited by the heterogeneous contact between the lithium source and spent LFP. Herein, polyacrylonitrile (PAN) was selected as the additive to facilitate the intimate contact between the lithium source and spent LFP. PAN displays a strong interaction with defective LFP, leading to the effective contact between spent LFP and the lithium replenishment agent. Moreover, PAN is favorable for the diffusion of lithium ions in the spent LFP lattice during the regeneration process. Therefore, the unevenly distributed FeLi defects in spent LFP are well-repaired. As a result, the regenerated LFP exhibits a high capacity of 155 mA h g–1 at 0.1 C and improved cycling stability with a capacity retention of ∼87% after 400 cycles at 1 C.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
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2025
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IF 9.8
Hao Pu,Xiaoming Zhu,Zhimin Zou,Chunhai Jiang
With the rapid development of energy storage devices and electric vehicles over the past decades, a large amount of lithium iron phosphate (LiFePO 4 , LFP) batteries are going to retire. Instead of recycling the low value Fe and P elements, direct regeneration of LiFePO 4 cathode has been recognized as the most cost-effective way to deal with the spent LiFePO 4 (S-LFP) batteries. However, the regeneration methods for S-LFP reported so far suffer from either using complex pre-oxidation and high temperature sintering steps, or expensive organolithium salt, which will inevitably increase the regeneration cost and give rise to additional environmental pollution. Herein, a deep eutectic solvent (DES) composed of lithium iodide, urea, and ascorbic acid (referred to as IUA) as prepared at 80 °C in ambient atmosphere is employed to regenerate S-LFP. This DES creates a Li-rich and reductive environment, enabling it to simultaneously supplement the deficient Li + ions, reduce Fe 3+ ions, and rectify the Fe Li “anti-site” defects in S-LFP under ambient pressure and optimally at 100 °C for 10 h. The regenerated LiFePO 4 demonstrates excellent electrochemical performance, with a high discharge capacity of 160 mAh g −1 at 0.1C and a remarkable capacity retention ratio of 85.8 % even after 400 cycles at 1C. Furthermore, the utilized IUA can be refreshed and reused for subsequent rounds of S-LFP regeneration. This characteristic renders the DES regeneration process both environmentally friendly and economically advantageous, thereby holding great promise for the practical recycling of S-LFP batteries.
研究领域:
材料科学
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环境科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Yun Luo,Fanbin Hu,Le Tian,Qingfeng Liu,Yi Fan,Yingjie Zhang,Zitong Fei,Qi Meng,Peng Dong
Direct regeneration is recognized as the most promising strategy for recycling spent LiFePO 4 (SLFP) due to its economic and environmental advantages. However, challenges persist in high-temperature solid-phase regeneration, including uneven lithium compensation from particle agglomeration and conflicting timing between lithiation and carbon coating. Therefore, a regeneration strategy is proposed utilizing a molecular fence and vapor deposition mechanism. Lithiation, vapor-deposited carbon coating, and in situ nitrogen doping are achieved through the synergistic effect of creatine and lithium stearate. Lithium stearate forms a molecular fence on SLFP surfaces, enhancing particle dispersion and uniform lithium replenishment. Below 300 °C, NH 3 released from creatine decomposition drives Li + insertion into the SLFP lattice to reduce Fe 3+ , completing lithiation. Subsequently, the generated small carbon-nitrogen molecules radicals undergo structural reorganization, forming a continuous conjugated structure that forms an in situ nitrogen-doped 3D conductive carbon network with topological defects. The heterocyclic and defective structures in the carbon coating modulate electron cloud distribution, creating additional active sites for electron transport and significantly improving conductivity. The regenerated LiFePO 4 delivers a discharge capacity of 146.2 mAh g −1 at 1 C and retains 95.83% capacity after 200 cycles. This strategy offers a viable pathway for high-efficiency, high-quality SLFP recycling.
研究领域:
材料科学
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环境科学
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化学工程
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能源化学
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固态化学
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电化学
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循环利用技术
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 36
·期 13
·2311553
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IF 29.4
Ruyu Shi,Nengzhan Zheng,Haocheng Ji,Mengtian Zhang,Xiao Xiao,Jun Ma,Wen Chen,Junxiong Wang,Hui-Ming Cheng,Guangmin Zhou
Direct regeneration of spent lithium-ion batteries has received wide attention owing to its potential for resource reuse and environmental benefits. The repair effect of direct regeneration methods undergoing heterogeneous repair process is usually inferior, while homogenous repair process plays a vital role to achieve satisfactory repair results. However, the practical applications of current homogeneous repair methods are challenged by the complex operations and relatively high costs owing to the requirement of additional heating or pressurization. Herein, this work proposes a simple strategy to achieve homogeneous repair of spent cathode materials under relatively mild conditions by uniformly precoating lithium source at room temperature and atmospheric pressure. Followed by annealing, highly degraded LiNi 0.83 Co 0.12 Mn 0.05 O 2 with severe Li deficiency and irreversible phase transition is repaired to have an initial capacity of 181.6 mAh g -1 and capacity retention of 80.7% after 150 cycles at 0.5 C. The lithium source used in this strategy is from the spent lithium anode. Moreover, this strategy is suitable for the direct regeneration of various layer oxide cathode materials with different failure degrees. This work provides both theoretical guidance and practical examples for the straightforward, effective, and universally applicable direct regeneration methods.
研究领域:
材料科学
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电化学
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能源存储
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可持续技术
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电池回收
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）