JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Haozheng Hu,Yaochun Yao,Xianghao Meng,Yin Li,Keyu Zhang,Shaoze Zhang,Yusong Yang,Yanqiu Xu,Junxian Hu
With the growing retirement of lithium iron phosphate (LiFePO 4 ) batteries, advanced recycling strategies are garnering widespread attention for resource sustainability. However, key issues such as high costs and improper disposal of hazardous waste urgently need to be addressed. Therefore, this paper proposes a systematic, green, and sustainable recycling process for spent LiFePO4 batteries. This method employs potassium pyrosulfate as a leaching agent to replace traditional inorganic acids, thereby reducing the negative environmental impact. Under optimal experimental conditions, the lithium (Li) leaching rate reaches 98.33 %, while the iron (Fe) leaching rate remains below 0.5 %, demonstrating high selectivity. The leaching process of LiFePO 4 in potassium pyrosulfate-hydrogen peroxide aqueous solution follows an Avrami kinetic model: l n k + n l n t = ln ( − ln ( 1 − x ) ) with an apparent activation energy of 18.69 kJ mol-1. This process is limited by both chemical and diffusion reactions. The recovered products, lithium carbonate and iron phosphate are utilized to synthesize regenerated LiFePO 4 . Compared to waste LiFePO 4 and fresh LiFePO 4 , the regenerated LiFePO 4 exhibits good electrochemical performance. Finally, an economic analysis reveals that the designed regeneration pathway possesses significant recovery value potential. This study proposes an efficient, economical, and sustainable closed-loop recycling technology for used lithium-ion batteries, facilitating resource recovery and environmental protection.
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DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Mingli Xu,Chen Wu,Fengxue Zhang,Yanhui Zhang,Jiaxin Ren,Chengyi Zhang,Xuanze Wang,Li Xiao,Olivier Fontaine,Jiangfeng Qian
Conventional metallurgical technologies for recycling cathode materials from retired Li-ion batteries go against carbon neutrality owing to massive material input and energy consumption. Although featuring with simplified process, direct regeneration technology still fails to bypass high-temperature driving forces for Li + compensation of degraded cathodes. Herein, chemical re-lithiation strategy mediated by ferrocene is proposed to directly regenerate the Li-deficient spent cathodes. Ferrocene and its derivatives, the so-called p-type redox mediators, can be oxidized spontaneously from neutral molecules to stable cations under ambient conditions, allowing them to function as electron donors . Meanwhile, lithium salts serve as Li + donors to ensure charge neutrality of the cathode lattice. The effects of solvation and substituent are thoroughly investigated to precisely regulate the potential of a series of ferrocene-based reductants. Chemical re-lithiation is driven thermodynamically by the intrinsic potential gap between ferrocene and degraded cathodes, thus fundamentally realizing a rapid lithiation reaction (taking less than 20 min at 25 °C), while avoiding the involvement of high-temperature operation. Diverse characterizations have been performed to explore the Li + -electron concerted re-lithiation mechanism. The regenerated LiFePO 4 cathode demonstrated comparable Li + storage capability to commercial cathode. Life-cycle analysis verifies the economical and environmental superiority of our chemical re-lithiation strategy to metallurgy in practical industry. The thermodynamically spontaneous chemical re-lithiation provides competitive options for greener recycling of retired batteries in the future.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yuhao Zuo,Shao-dong Zhou,Yuchen He,Ke-Jun Wu
The use of Fe 3+ salts for leaching spent LiFePO 4 (LFP) batteries is gaining attention due to its mild, eco-friendly conditions. However, efficient Fe/Li separation remains challenging, as precipitation causes Li loss or impurity introduction, and conventional solvent extraction offers low Li efficiency (∼80 %) and complex processes. This study employed data mining and theoretical analysis to rapidly identify a synergistic P204/N235 extraction system. A closed-loop process coupling H 3 PO 4 stripping and FePO 4 precipitation was developed, achieving 99.45 % Fe removal and only 1.25 % Li loss in a single extraction stage. The Fe/Li separation factor reached 14,243. During stripping, Fe recovery reached 95 % in one stage. The aqueous phase over 10 stripping cycles was reused for FePO 4 preparation, and the raffinate was retained for Li recovery. This integrated approach enables efficient Fe/Li separation and high-value resource utilization from LFP leachates.
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高影响因子
Materials Today Physics
·
2022
·
IF 11.021
Yanqing Wang,Rui Xu,Bowen Xiao,Dong Lv,Yu Peng,Yun Zheng,Yanghuan Shen,Jingchao Chai,Xiaohua Lei,Shiyu Luo,Xinyi Wang,Xinmiao Liang,Jiwen Feng,Zhihong Liu
Solid-state polymer electrolytes have recently drawn intense attention as alternatives to traditional liquid electrolytes in lithium batteries due to their high energy-density and reliable safety. Unfortunately, current all-solid-state polymer electrolytes suffer from the low ionic conductivity , limiting the power density of energy storage batteries . Here, we propose a deep-eutectic electrolyte, formed directly by the interaction between poly (1,3-dioxolane) and lithium salt without other auxiliary solvents. The ionic conductivity of the designed deep-eutectic polymer electrolyte can approach to 1.5 × 10 −5 S/cm at ambient temperature, which is twenty times higher than that of polyethylene oxide-based electrolytes. Specifically, solid-state NMR verifies the interaction between oxygen in poly (1,3-dioxolane) and lithium ion . The LiFePO 4 /Li battery assembled with deep-eutectic polymer electrolyte delivers a discharge capacity of 139.6 mAh/g at 0.1 C and a capacity retention of 90% after 200 cycles at 0.2 C. Pouch LiFePO 4 /Li batteries also present excellent safety performances. This finding provides a new approach for materials engineering of polymer electrolytes for advanced lithium batteries.
研究领域:
材料科学
·
能源存储技术
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高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2019
·
IF 6.309
Xuelian Fu,Yuchao Li,Chengzhu Liao,Weiping Gong,Mingyang Yang,Robert Kwok Yiu Li,Sie Chin Tjong,Zhouguang Lu
Low ionic conductivity and large interfacial impedance between the electrode and electrolyte are the main bottleneck issues of the current solid electrolytes . In this study, a novel 3D hierarchical solid electrolyte was developed to tackle the large interfacial impedance problem. A flexible polyethylene oxide/lithium chlorate (PEO/LiClO 4 ) was in-situ formed inside the 3D porous Li 6.28 La 3 Zr 2 Al 0.24 O 12 (LLZAO) network by simply using a cleanroom wiper as the template. The obtained 3D LLZAO-PEO/LiClO 4 composite solid electrolyte exhibited a high ionic conductivity of 2.25 × 10 −5 S cm −1 at 30 °C, being 30.7 times higher than that of pristine PEO/LiClO 4 electrolyte. The improved ionic conductivity was attributed to the 3D porous LLZAO structure with continuous fast ion transport pathways. In addition, the 3D LLZAO network can effectively inhibited the growth of lithium dendrite , leading to excellent stability and desirable safety during lithium stripping/plating cycling. Furthermore, the all-solid-state LiFePO 4 /Li battery system based on the obtained 3D LLZAO-PEO/LiClO 4 electrolyte showed a high initial discharge specific capacity of 143.8 mAh·g −1 and a high capacity retention of 86% after 200 cycles at 60 °C. This 3D composite solid electrolyte design is very effective in reducing the interfacial impedance and provides a solution for the further development of high-performance solid electrolyte for all-solid-state rechargeable batteries.
研究领域:
材料科学
·
电化学
·
电池技术
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Advanced Energy and Sustainability Research
·
2024
·
IF 6.2
Jiancong Cheng,ChuTao Wang,Kun Wang,Kai Lan,Chen Li,Jingmin Fan,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
Thick electrodes represent an effective approach for augmenting energy density of batteries. However, their increased thickness invariably leads to longer electron and ion transport distance, limiting the utilization of active material and hindering practical application. Herein, an electron-conducting-enhanced and ion-conducting-enhanced strategy is presented for fabricating ultrahigh loading electrodes via constructing an interlaced 3D network. Carbon nanotubes (CNTs) serve as extended electron pathways. Different from the polyvinylidene fluoride binder which needs to be dissolved into molecules for preparing electrode, polytetrafluoroethylene (PTFE), however, exists as a separate phase inside the electrode, thus can become the extended pathways for electrolyte elongating due to its strong affinity to organic electrolyte. Note that based on the synergistic effect between CNT and PTFE, the latter can exhibit a form of long-distance extension fibers rather than agglomeration. Finally, a LiFePO 4 electrode with a record-high loading of 141 mg cm −2 is successfully prepared. This electrode exhibits outstanding area capacity (20.7 mAh cm −2 at 0.2 C) and cycling stability with impressive energy density of 224 Wh kg −1 and 517 Wh L −1 in a full cell (graphite anode). The findings present a novel strategy for achieving high energy density in lithium-ion batteries using existing material systems.
研究领域:
材料科学
·
能源存储
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2012
·Vol. 159
·期 3
·A305
·
IF 2.59
Chang Su,Guoqiang Lu,Lihuang Xu,Cheng Zhang
In this work, the spindle-shaped LiFePO4 coating with carbon layer (C-LFP) was successfully synthesized in glycerol solvent assisted by a mild heat-treatment at 600°C for 2 h. Then camphorsulfonic acid doped polyaniline (PANI-CSA) as the conductive polymer was compound with C-LFP to prepare C-LFP/PANI-CSA composite. The morphology, crystal structure and charge-discharge performance of the prepared samples were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and galvanostatic charge-discharge testing. The results showed that the reactant concentration seriously affected the microstructure and electrochemical properties of the resulting LiFePO4 cathodes in lithium ion batteries. And a spindle-shaped LiFePO4 with suitable size has been successfully synthesized at the moderate reactant concentration of 0.5 M. After modified with PANI-CSA, the resulted C-LFP2/PANI-CSA composite cathodes displayed a significantly improved specific capacity and rate capability. And specially, that the C-LFP/10%PANI-CSA composite exhibited the best performance with an initial discharge capacity of 165.3 mAh·g−1 at a constant current of 0.1 C. Electrochemical impedance measurements also demonstrated that the coating of polyaniline significantly decreased the charge-transfer resistance of C-LiFePO4 electrodes.
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Advanced Energy Materials
·
2026
·
IF 25.5
Tuan Wang,Fangbing Li,Enhao Xu,Jie Hu,Haijun Xia,Hao Wu,Wenlong Cai,Yun Zhang,Kaipeng Wu
The recovery of high-purity iron phosphate (FePO 4 ) from lithium extraction slag (LES) is crucial for achieving closed-loop recycling of spent LiFePO 4 /C. However, this process is significantly challenged by the difficulty in removing aluminum impurities due to the similar chemical behavior of Fe 3+ and Al 3+ . Guided by thermodynamic principles, we developed a three-stage purification process for deep aluminum removal, consisting of “selective leaching-precipitation-dissolution/recrystallization.” In the first stage, highly selective aluminum leaching (96.3% Al vs. 21.6% Fe) is achieved under mild acidic conditions, leveraging the thermodynamic preference for aluminum dissolution over FePO 4 . During the second stage, by utilizing the tendency of Fe 3+ to precipitate more readily as FePO 4 ·xH 2 O than Al 3+ , precise pH control enables 95.5% iron precipitation, with only 4.02% aluminum coprecipitation. The third stage involves an in situ dissolution/recrystallization, which promotes efficient iron recrystallization (95%) while further removing residual aluminum, reducing its content by over 50% from an already low level. This enhancement is attributed to the higher crystallization tendency of FePO 4 ·2H 2 O compared to AlPO 4 ·2H 2 O. Ultimately, battery-grade FePO 4 with an aluminum content below 300 ppm is obtained. This work provides an industrially viable strategy for the deep removal of aluminum and the high-value utilization of LES derived from spent LiFePO 4 /C.
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SOLID STATE IONICS
·
2019
·
IF 2.886
Jiang Zhou,Dongyun Zhang,Guanghan Sun,Chengkang Chang
Lithium-iron phosphate (LiFePO 4 ) monocrystalline platelets (LFP-P) with ac facet-preferred growing were obtained by a solvothermal method . Based on its anisotropy, a LiFePO 4 cathode (LFP-PM) with the b axis-oriented aligning was prepared by magnetic orientation. The structure, morphology and magnetic performance of the LFP-P were studied by X-ray diffractometry, scanning-electron microscopy, transmission-electron microscopy and superconducting quantum-interference device technologies. The LFP-P exhibited paramagnetic behavior and its b axis had the largest magnetic susceptibility , which made the LFP-P stack parallel to the magnetic field . It resulted in a higher lithium-ion diffusion coefficient of the LFP-PM (1.6855 × 10 −11 cm 2 s −1 ) compared with that of the LiFePO 4 cathode (LFP-PU) prepared without magnetic orientation (1.2538 × 10 −11 cm 2 s −1 ). The faster lithium-ion diffusion was contributed to a higher reversibility at 0.1 mV s −1 and higher discharge capacities of the LFP-PM at high rates ≥2 C. For the first time, LiFePO 4 monocrystalline platelets were made to align along b axis through magnetic orientation. It was proved to be an effective means of enhancing high rate performance.
研究领域:
材料科学
·
电化学
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高影响因子
VACUUM
·
2023
·
IF 4
Xiaoxiao Pan,Yuqing Sun,Shuxin Zhuang,Gaoxing Sun,Shengyu Jiang,Yan Ren,Yanfen Wen,Xiaodan Li,Feiyue Tu
The application of LiFePO 4 cathode material in the field of power lithium-ion batteries is seriously hampered by its poor rate performance that is triggered by its inherent poor electrical conductivity and low ion diffusion coefficient . Herein, an inexpensive and facile preparation method is developed to fabricate a novel nano-micro porous structural LiFePO 4 cathode using 30 nm carbon black and iron powder as direct raw materials. It is found that the added amount of carbon black is an important factor affecting the phase and morphology of the products. Optimizing the amount of carbon black, the LiFePO 4 cathode with the unique nano-micro porous structure and high specific surface area could be obtained. Such unique porous architecture with a high specific surface area can accelerate lithium-ion diffusion during charge/discharge to promote its rate performance. Meanwhile, the residual graphitized carbon derived from carbon black can not only enlarge the surface pseudocapacitance under high C rates but also enhance its electronic conductivity. Benefit from the suitable pseudocapacitive behavior and high Li + diffusion coefficient , the LFP-1.5 electrode exhibits a discharge specific capacity of 166.27 mAh/g at 0.1C and 124.95 mAh/g at 20C, indicating prominent discharge specific capacity and excellent high-rate charge/discharge capability.
研究领域:
材料科学
·
储能技术
·
电化学
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DOI
高影响因子
Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·137
·
IF 36.3
Lan Yuanqi,Wen Jianfeng,Zhang Yatian,Lan Xuexia,Song Tianyi,Zhu Jie,Peng Jing,Yao Wenjiao,Tang Yongbing,Cheng Hui-Ming
Simultaneously repairing the degraded crystal structure and reconstructing the damaged carbon coating in spent LiFePO 4 cathode enables superfast lithium-ion diffusion kinetics and produces a stable cathode–electrolyte interface.
The regenerated LiFePO 4 cathode delivers remarkable rate capability, low-temperature performance and compatibility in solid-state batteries.
The proposed direct regeneration approach has high economic and environmental benefits compared to hydrometallurgical and conventional direct recycling methods.
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Fangbing Li,Tuan Wang,Jinxuan Chen,Jie Hu,Haijun Xia,Enhao Xu,Hong Wu,Yun Zhang,Kaipeng Wu
The continuous accumulation of spent LiFePO4 (S-LFP) and LiMn2O4 (S-LMO) cathodes demands efficient and sustainable recycling strategies, as conventional hydrometallurgical processes rely heavily on external redox agents, increasing the cost and environmental burden. This study proposes an innovative synergistic leaching process that enables the upcycling of mixed spent LFP and LMO into high-voltage LiFexMn1–xPO4 (LFMP) without any additional redox agents. We established a multireaction feedback system centered on self-redox in a sulfuric acid medium through the design of multiple sets of experiments for verification, achieving highly efficient leaching of Li (99.5%), Mn (99.2%), and Fe (99.6%) under optimized conditions (H2SO4–metal molar ratio of 2, liquid–solid ratio of 5, temperature of 30 °C, and time of 120 min). The leachate was subsequently converted to an Fe–Mn–P composite precursor and then upcycled into LFMP. The regenerated LiFe0.4Mn0.6PO4 cathode delivers a remarkable energy density of 557.67 Wh kg–1 at 0.2 C, significantly surpassing that of commercial LFP and LMO. Electrochemical analysis confirmed that the diffusion capability of Li+ within the Mn reaction region is critical for the unlocking of energy density for LFMP electrodes. Economic and environmental assessments further confirmed the superior profitability (2.24 $ kg–1) and reduced greenhouse gas emissions of this synergistic upcycling route, demonstrating its potential as a sustainable and economically viable strategy for recycling multisource spent cathodes into new-generation high-energy-density materials.
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