ACS Nano
·
2026
·
IF 17.3
Xia Qiuli,Yang Chuanwei,Zhang Danni,Li Zhong,Li Min,Li Jiaxin,Tong Linlin,Guan Xianjun,Jiang Tianqi,Fan Yongqiang,Gu Tingyue,Wang Fuhui,Xu Dake
The sustainable recycling of spent lithium iron phosphate
(LiFePO 4 ) batteries via bioleaching is critically important
yet often
constrained by low processing capacity and severe microbial oxidative
stress. Herein, we report a highly efficient biocatalytic strategy
utilizing Gluconobacter oxydans as
a whole-cell biocatalyst for the leaching of spent LFP batteries.
We demonstrate that the addition of 25 mM ascorbic acid (AA) dramatically
enhances the catalytic performance of this microbial system, achieving
a high lithium extraction yield of 92.7% within 7 days at a pulp density
of 10.0 g L –1 . Transcriptomic and biochemical analyses
elucidate a novel synergistic catalytic mechanism: AA not only alleviates
intracellular oxidative stress to sustain microbial catalyst but also
actively participates in a pyrroloquinoline quinone (PQQ)-mediated
extracellular redox cycle. In this cycle, the reduction of PQQ by
AA and its subsequent reoxidation by O 2 generate H 2 O 2 . Under mild acidic conditions (pH ∼4),
these H 2 O 2 preferentially drive the catalytic
oxidation of LiFePO 4 to FePO 4 , thereby significantly
facilitating Li release. The dissolved Li was further recovered from
bioleachate as Li 3 PO 4 , while the FePO 4 -rich residues showed effective dye–removal activity, demonstrating
residue valorization potential. This work unveils the dual function
of AA in fortifying the microbial catalyst and driving mineral oxidation,
presenting a practical and economically viable strategy for the integrated
recycling of spent LFP batteries.
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高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Yuelin Kong,Shuaipeng Hao,Yaqi Liao,Yudi Shao,Le Hu,Wei Liu,Yuanguang Xia,Wen Yin,Jingwei Xiang,Yunhui Huang,Lixia Yuan
The LiFePO 4 batteries are expected to face a significant wave of retirement in the coming years. This necessitates the establishment of a comprehensive and environmentally friendly recycling system for spent LiFePO 4 batteries. The traditional hydrometallurgical and pyrometallurgical methods involve high costs and serious pollution. This work provides a more efficient and environmentally benign alternative by repairing spent LiFePO 4 through a citric acid-LiCl deep eutectic solvent (DES). The citric acid and LiCl form a molten state through hydrogen bonding at lower temperatures, enabling the ambient-pressure repair. The LiCl acts as a Li source to replace the lost Li. The citric acid donates electrons to reduce Fe 3+ to Fe 2+ , reducing electrostatic repulsion to facilitate Fe to return to its original lattice site, thereby eliminating Fe-Li anti-site defects and promoting the insertion of Li + into the lattice. Remarkably, this method eliminates the strict requirement for Li/Fe molar ratio control, making it applicable to spent LiFePO 4 batteries with varying degradation levels. The regenerated LiFePO 4 shows great electrochemical performance with a discharge capacity of 158.3 mA h g −1 at 0.5 C, with a capacity retention of 82.8% after 600 cycles. Notably, the DES demonstrates recyclability and stable regeneration efficiency, while its eco-friendly nature further enhances the economic viability and industrial potential of this process.
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ENERGY & FUELS
·
2026
·
IF 6
Feifan Li,Min Zhang,Zhen Zheng,Lei Li
With the booming development of the lithium-ion battery industry, there is an urgent need to develop an effective recycling method for lithium iron phosphate (LiFePO4, LFP) cathode materials of spent lithium-ion batteries. Herein, a direct hydrothermal regeneration strategy for industrial LFP black mass using low-cost glucose as a multifunctional agent is proposed. Under hydrothermal conditions, glucose not only serves as a reductant to convert FePO4 back to the LiFePO4 phase and heal Li–Fe antisite defects but also in situ generates a uniform carbon coating via hydrothermal carbonization. The regenerated LFP cathode delivers a high specific capacity of 153.16 mAh g–1 at 0.1 C and exhibits outstanding cycling stability with 89.27% capacity retention after 300 cycles at 0.5 C. A comprehensive techno-economic analysis further reveals that this glucose-assisted hydrothermal route offers significant economic and environmental advantages over conventional methods, presenting a promising scalable solution for sustainable battery recycling.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yangyang Li,Shurong Xu,Shoujing Mao,Wenxin Liu,Quan Yuan,Ying Wu,Xin Guo,Yihong Tong,Zhongkai Li,Danya Li,Jun Liu
The continuous accumulation of spent LiFePO 4 cathodes underscores the urgent need to develop sustainable and economically viable recycling technologies. An efficient solid-state regeneration strategy is established to realize lithium replenishment and defect reconstruction by a simple process to reduce spent LiFePO 4 only through thermal decomposition of L-cysteine. Acting concurrently as a reductant, carbon precursor, and N/S dopant, L-cysteine facilitates lattice reconstruction while forming a uniform N/S co-doped carbon coating that enhances the cathode electronic conductivity. DFT calculations further reveal that the regeneration process preferentially stabilizes the (010) facet by significantly reducing its surface energy, thereby exposing a low-energy Li + -conducting plane that accelerates ion migration. The regenerated LiFePO 4 demonstrates a high discharge capacity up to 137.78 mAh g −1 even at 1C and maintains 121.5 mAh g −1 after 500 cycles, corresponding to an excellent capacity retention of 86%. This work offers a feasible and economically competitive strategy to regenerate LiFePO 4 not only with N/S co-doped carbon coating, but also with (010) exposure facet, which impart directly regenerated LiFePO 4 with enhanced electronic conductivity and accelerated ion transport to exhibit excellent lithium-storage performances.
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高影响因子
Energy Storage Materials
·
2026
·
IF 19.3
Xuan Cao,Wei Mao,Jingnan Yuan,Shaochun Tang
Thermal pretreatment is a key step for purifying spent LiFePO 4 (LFP) cathode materials by removing surface residues, but the microstructural damage in the spent LFP powder has been rarely studied. In this work, we found that thermal pretreatment inflicts severe secondary damage by forming inert Fe 2 P 2 O 7 phases and introducing a large number of Fe/Li antisite defects; this damage is further confirmed as the root cause of the intrinsic failure of conventional lithium-replenishment strategies in LFP regeneration. To eliminate the thermal damage induced by pretreatment, an interface-selective lithium anchoring (ISLA) strategy is proposed based on the newly identified mechanism. The ISLA strategy constructs functionalized interfaces in which abundant functional groups act as selective sites to anchor and disperse lithium, thereby enabling in situ reconversion of Fe 2 P 2 O 7 to LiFePO 4 and effective reduction of Fe/Li antisite defects. The regenerated LFP exhibits high-rate capability, delivering 121.8 mA h g -1 at 10 C, and excellent cycling stability, retaining 72.7% of its capacity after 1500 cycles. This work provides a scalable and sustainable route for regenerating spent LFP cathode materials with reduced energy demand and carbon footprint.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Ming Zhou
LiFePO 4 battery is one of the three mainstream cathode materials for Lithium-ion batteries, with a market share of approximately 60%. With the rapid development of electric vehicles, plenty of spent LiFePO 4 batteries will inevitably accumulate, causing a waste of resources and environmental problems. Thus, spent LiFePO 4 recycling has become increasingly important. During the recovery process, mixing spent LiFePO 4 black powder and H 2 SO 4 resulted in a leaching solution containing complex compositions, such as Li, Fe, P, Co, Ni, Cu, Mg, Mn, and Al. The P and Fe elements are recovered through the FePO 4 precipitation. After solid-liquid separation, 5-6 g/L of Li and other accompanying impurities are retained in the mother liquor. The Li-bearing solution above is purified using the two-step precipitation method. Then, battery grade LiOH·H 2 O is successfully synthesized by using the Li 2 SO 4 causticizing process. The effects of operating parameters, including reaction temperature, excess coefficient of NaOH, Li concentration, and reaction time are investigated in detail. Under the optimal conditions, 96.18% of the Li in the initial concentrated Li 2 SO 4 solution is converted to LiOH solution by the reaction (Li 2 SO 4 + 2NaOH + 10H 2 O → 2LiOH + Na 2 SO 4 ·10H 2 O). Meanwhile, the Li content in Na 2 SO 4 ·10H 2 O can be controlled at around 0.2%, and the Li recovery rate for the process of Na 2 SO 4 by-product prepared by Na 2 SO 4 ·10H 2 O is as high as 98.30%. This study is expected to provide valuable insights into the high value-added recovery of Li from spent LIBs.
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高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Zhao Zhao,Yan Li,Ziyu Chen,Chengzong Li,Haibin Zeng,Chengming Du,Tao Li
Traditional recycling technologies for spent lithium iron phosphate (LiFePO 4 , LFP) usually suffer from issues such as complex procedures, heavy chemical consumption, and limited economic viability. Herein, we propose a method combining FeCl 3 leaching and spray pyrolysis for the high-value-added recycling of spent LFP. Using FeCl 3 as leaching agent, over 99 % of Li is selectively leached out within 30 min with a solid-liquid ratio up to 300 g L −1 . The resulting leaching residue (FePO 4 ) serves as a precursor for the synthesis of new LFP. Subsequently, the Li and Fe-containing leachate undergoes a spray pyrolysis process, yielding a pyrolysis powder comprising LiCl and Fe 2 O 3 . Through a water-leaching procedure, the separation of LiCl and Fe 2 O 3 is achieved based on their distinct solubility in water. The resulting high-purity LiCl solution and Fe 2 O 3 residue are directly utilizable for producing battery-grade Li 2 CO 3 and LFP cathodes, respectively. LFP/C cathodes, synthesized using the recovered Li 2 CO 3 and FePO 4 precursor, exhibit an impressive 99.8 % capacity retention after 200 cycles at a 1C rate. This method holds great economic and environmental benefits by producing high-value-added products while avoiding the consumption of acids or alkalis.
研究领域:
材料科学
·
环境工程
·
化学工程
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高影响因子
ACS Nano
·
2025
·
IF 16
Xuan Cao,Wei Mao,Yingze Song,Shaochun Tang
Most current regeneration methods are predicated on the assumption of uniform degradation, making them inadequate to precisely address the structural disparities and defect heterogeneity among particles, thereby limiting their applicability for large-scale regeneration of industrial LiFePO4 black mass. In this work, we propose a scalable and simplified solid–liquid hybrid strategy that enables efficient regeneration of kilogram-scale, heterogeneously degraded LiFePO4 cathodes at room temperature under laboratory conditions. The approach leverages localized interfacial redox processes at room temperature to achieve precise lithium compensation at the particle level. However, atomic-resolution analyses reveal that lithium replenishment alone is insufficient to repair Fe/Li antisite defects within the crystal lattice, particularly in mildly delithiated particles (<5%), where the migration energy barrier reaches 2.78 eV, thus impeding deep structural recovery. To overcome this limitation, a subsequent thermal activation step is incorporated to eliminate deep-seated antisite defects and enable complete lattice reconstruction. This combined approach leads to multiscale structural recovery, allowing the regenerated material to achieve a reversible specific capacity of 114.2 mA h g–1 at 10.0 C and retain 79.2% of its capacity after 1500 cycles. These findings validate the method’s wide applicability to structurally complex degradation scenarios and offer mechanistic and practical insights into scalable regeneration of high-performance electrodes.
研究领域:
材料科学
·
电化学
·
能源存储
·
再生技术
·
纳米材料
·
固态化学
·
电池回收
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
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
·
环境科学
·
化学工程
·
能源化学
·
固态化学
·
电化学
·
循环利用技术
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高影响因子
JOURNAL OF PORPHYRINS AND PHTHALOCYANINES
·
2018
·Vol. 22
·期 12
·1072-1081
·
IF 1.217
Yuanyuan Su,Feifei Xu,Ruiqiong Wang,Ronglan Zhang,Jianshe Zhao
The monodispersed LiFe 1 − x M x PO 4 /C [ x ≈ 0.0040; M = Mn 2 + , Co 2 + , Ni 2 + , Cu 2 + , Zn 2 + ] nanocomposites obtained by LiFePO 4 modified with binuclear metal aminophthalocyanines (M 2 (PcTa) 2 O and M 2 (PcTa) 2 C(CF 3 ) 2 ) are utilized as positive electrode materials for lithium ion batteries. The preparation method for these nanocomposites is a controllable solvothermal method using a mixture of ethylene glycol and N , N -dimethylformamide as the solvent. The microstructure and electrochemical properties of the different nanocomposites are discussed and compared. The results show that the LiFePO 4 samples modified with M 2 (PcTa) 2 C(CF 3 ) 2 can improve the initial discharge specific capacity of the lithium ion battery up to 154.2 mAh.g − 1 at the rate of 0.1 C, and 93.5% of the initial discharge capacity could be retained after 50 cycles. This research shows that the proposed process can enhance the electrochemical performance of high power LiFePO 4 for lithium ion batteries.
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高影响因子
Journal of Physical Chemistry C
·
2012
·
IF 4.805
Jing Su,Xing-Long Wu,Chun-Peng Yang,Jong-Sook Lee,Jaekook Kim,Yu-Guo Guo
A general and efficient hydrothermal strategy combined with a high-temperature carbon-coating technique has been developed for large scale synthesis of self-assembled LiFePO4/C nano/microspheres employing the biomass of phytic acid as a novel and eco-friendly phosphorus source. The LiFePO4/C nano/microspheres are investigated by SEM, TEM, EDS, XRD, Raman spectroscopy, and electrochemical techniques. A reasonable assembly process of the hierarchical structure is proposed on the basis of time-dependent experimental results. Because of the unique structure, the LiFePO4/C nano/microspheres show a high tap density of 1.2 g cm–3, a high reversible specific capacity of 155 mA h g–1 at 0.1 C, as well as excellent rate capability and cycling performance, exhibiting great potential as superior cathode materials in lithium ion batteries. The approach for the preparation of LiFePO4 by using PA as the phosphorus source may open new prospects for utilization of biomass to produce high performance cathode materials for lithium ion batteries.
研究领域:
材料科学
·
储能
·
纳米技术
·
电化学
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Peiwen Liu,Yannan Zhang,Peng Dong,Yingjie Zhang,Qi Meng,Siyuan Zhou,Xuan Yang,Mingyu Zhang,Xi Yang
Direct regeneration has been widely applied in recovery of LiFePO 4 batteries. However, excess residual carbon and inherent low electronic and ionic conductivity of spent LiFePO 4 /C cathode materials lead to the reduction of electrochemical performance. Herein, a facile and simple regeneration process of pre-oxidation and vanadium doping is developed to regenerate LiFePO 4 /C cathode materials . Pre-oxidation was applied to remove excess carbon at 500 °C for 3 h in air. Vanadium doping was applied to improve electronic and ionic conductivity of regenerated cathode materials. Among the regenerated cathode materials, the 3 mol% V doped sample possesses discharge capacity of 134.3 mAh/g after 200 cycle at 1C with the discharge capacity retention of 99.1%. At 2, 5, 10C, the discharge capacities are 134, 124.1, 111.5 mAh/g, respectively. The vanadium doping regeneration process with oxidation pre-oxidation is simple, and feasible to be applied in the recovery of spent LiFePO 4 cathode materials.
研究领域:
材料科学
·
能源存储与转换
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高影响因子
危险品化学品经营许可证（带存储）