ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Shujie Tang,Mei Zhang,Min Guo
A new type of deep-eutectic solvents (DESs), consisting of ethylene glycol (EG) and sulfosalicylic acid dihydrate (SAD), were designed for efficient leaching valuable metals from cathode active materials (LiCoO2 and Li14.8Ni1.7Co8.5MnO30.5) of spent lithium-ion batteries (LIBs) for the first time. The as-prepared DESs possessed strong coordination ability and low viscosity, which were suitable for metal extraction. The influences of experiment parameters on extraction of Co and Li were systematically investigated, and the leaching mechanism and kinetics were elucidated in detail. Under the optimal conditions, the leaching efficiencies of Co and Li from pure LiCoO2 reached 93.5% and 98.3%, while those of Co, Ni, Mn, and Li achieved 94.8%, 99.1%, 100%, and 100% from the spent Li14.8Ni1.7Co8.5MnO30.5, respectively. Results revealed that the Li+ ions located in the interlayer of layered LiCoO2 were replaced by H+ ions and entered into solution, while Co3+ ions in the skeleton structure were reduced and coordinated by EG and sulfosalicylic acid (SA) to form four soluble Co2+–SA complexes, realizing synergistic and efficient leaching of Li and Co from the LIB cathode active material. Moreover, Co and Li leaching kinetics conformed to the shrinking core model, in which the interfacial chemical reaction was the limiting step, and the apparent activation energies were separately about 77.38 and 79.54 kJ/mol.
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
高影响因子
Journal of Energy Chemistry
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2024
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IF 14
Shuzhe Yang,Hao Luo,Yukun Li,Qingqing Gao,Hui Li,Hongwei Cai,Xiaodan Li,Yanfen Wen,Yujin Tong,Tiefeng Liu,Mi Lu
Traditional pyrometallurgy and hydrometallurgy processes primarily focus on the recovery of valuable metals (Co, Ni, etc.) from spent lithium-ion batteries. However, these methods are not economical for recycling cheap LiFePO 4 . Herein, a synergistic thermal-decomposition and electric-drive strategy is proposed to recover the whole spent LiFePO 4 electrode by in-situ recovering the inactive lithium (dead lithium and trapped interlayer lithium). Firstly, the organic components in the dense solid electrolyte interface (SEI) are effectively decomposed through thermal-decomposition processing, exposing the dead lithium encapsulated within the SEI and recovering the electron channels between the dead lithium and graphite. Leveraging the difference between the Gibbs free energy of the dead lithium and graphite as the driving force facilitates the dead lithium inserting into the anode. Then, fully utilizing the remaining discharge capacity of the spent LiFePO 4 cell, the inactive lithium is reinserted into LiFePO 4 lattice during the electric-drive process. Consequently, the reactivated lithium content increases by more than 16%, reaching a capacity of 134.2 mA h g −1 compared to 115.2 mA h g −1 from degraded LiFePO 4 , allowing for effective participation in the subsequent cycling. This work provides new perspectives on highly profitable cycles with low energy and material consumption and a low carbon footprint.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Ruiqi Che,Sha Cheng,Cheng Huang,Ming Liu,Zhongao Chen,Jin Han,Wen Chen,Pengchao Zhang
Lithium dendrites, growing during the charging and discharging processes, can pierce the separators and lead to internal short circuits, which is one of the main factors resulting in thermal runaway of lithium metal batteries (LMBs). In this work, we developed a poly(vinylidene fluoride) (PVDF)-based Janus separator with an ultrathin polypyrrole (PPy) layer towards efficiently suppressing lithium dendrite growth. The PPy layer with thickness of approximately 200 nm has Pyrrole-N with lone pairs of electrons, which can act as nucleation sites for lithium ions. As a result, lateral lithium deposition can be achieved on the anode, thus preventing the lithium dendrites from piercing the separators. Stable stripping/plating performance over extended cycling and a capacity retention rate of 76.8% after 1000 cycles have been achieved in the Janus PVDF/PPy separator-based Li//Li symmetric cells and Li//LiFePO 4 half cells, respectively. The development of Janus separators with conductive polymer layers presents a promising solution for improving the safety and electrochemical performance of LMBs.
研究领域:
材料科学
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能源存储
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产品关联
DOI
高影响因子
Advanced Energy Materials
·
2018
·Vol. 8
·期 16
·1702374
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IF 21.875
Yijie Liu,Chao Li,Bojie Li,Hucheng Song,Zhu Cheng,Minrui Chen,Ping He,Haoshen Zhou
Solid-state Li batteries using Na + superionic conductor type solid electrolyte attracts wide interest because of its safety and high theoretical energy density. The NASCION type solid electrolyte LAGP (Li 1. 5 Al 0.5 Ge 0.5 P 3 O 12 ) shows favorable conductivity as well as good mechanical strength to prevent Li dendrite penetration. However, the instability of LAGP with Li metal remains a great challenge. In this work, an amorphous Ge thin film is sputtered on an LAGP surface, which can not only suppress the reduction reaction of Ge 4+ and Li, but also produces intimate contact between the Li metal and the LAGP solid electrolyte. The symmetric cell with the Ge-coated LAGP solid electrolyte shows superior stability and cycle performance for 100 cycles at 0.1 mA cm −2 . A quasi-solid-state Li–air battery has also been assembled to further demonstrate this advantage. A stable cycling performance of 30 cycles in ambient air can be obtained. This work helps to achieve a stable and ionic conducting interface in solid-state Li batteries.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2017
·Vol. 135
·期 11
·46020
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IF 1.86
Shan Jiang,Wei Wang,Tianya Huang,Jie Ma,Yonghong Ding,Qiang Yu
Terpolymer poly(α-methylstyrene- co -glycidyl methacrylate- co -4-acryloyl tetraphenylethylene) (PAGT) was synthesized by radical copolymerization using α-methylstyrene, glycidyl methacrylate, and trace fluorescent monomer 4-acryloyl tetraphenylethylene. Thermal decomposition of α-methylstyrene constitutional units in copolymer chains is known to produce macromolecular radicals at temperatures exceeding 90 °C, which may be melt-grafted to polypropylene (PP) without other initiators by means of extrusion. In this study, the PP- g -PAGT microporous material was prepared by casting and stretching. The structure and properties of the PAGT were characterized by Fourier transform infrared spectroscopy, 1 H-nuclear magnetic resonance, and thermogravimetic analysis. The grafting degree and rheological properties proved that the PAGT chains were successfully grafted onto the PP. The uniformity of the PAGT in the PP- g -PAGT was observed using a spectrofluorophotometer. The polarity of the cast membrane was characterized by the water contact angle. The results showed that the PAGT evenly grafted onto the PP, and the polarity and hydrophilicity of the cast membranes were improved. The microporous structure of the separator was observed via scanning electron microscopy. Testing of the performance of the lithium battery showed that the impedance decreased and the ionic conductivity increased with the introduction of PAGT onto PP. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46020.
研究领域:
材料科学
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高分子化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2019
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IF 5.383
Weishang Jia,Tao Chen,Ying Wang,Siji Qu,Zeyu Yao,Yuchi Liu,You Yin,Wei Zou,Fu Zhou,Jingze Li
Lithium metal is an ideal anode material for lithium battery thanks to its ultra-high specific capacity and lowest redox potential . However, uncontrollable growth of lithium dendrites hinders its application due to local aggregation of lithium ions and anisotropic growth of lithium metal driven by uneven electric field distribution. Here a strategy is proposed to address this issue via utilizing porous equipotential body decorated with heterogeneous nucleation sites as advanced three-dimensional current collector. The conductive network of carbon nanofibers is recognized as a porous equipotential body, where the interior electric filed is zero due to the well-defined electric field shielding effect. In addition, copper nanoparticles as heterogeneous nucleation sites are uniformly anchored on carbon nanofibers, which guide lithium deposition evenly. As a result, lower impedance and higher Coulombic efficiency (∼97%) are achieved in modified lithium-copper cell. In particular, the cycling lifetime of modified symmetric lithium-lithium cell is expanded up to 500 cycles at extremely large current density of 50 mA cm −2 .
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
ACTA MATERIALIA
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2024
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IF 8.3
Jinping Mu,Xiaohui Li,Rui He,Lijing Sun,Xue Bai,Lihui Zhang,Xi Zhang,Zhenfa Liu,Jing Gao,Aijia Wei
High-voltage (5-V) lithium–ion batteries (LIBs) have garnered substantial interest due to their superior energy density. Nevertheless, the unstable interphase of high-voltage LIBs can cause electrolyte decomposition, electrode collapse, transition metal dissolution, and lithium dendrite growth during cycling, which impedes their widespread commercial use. To mitigate these challenges, various alkali-metal phosphates were incorporated into a carbonate-based electrolyte as film-forming additives, aiming to improve the electrochemical performance of LiNi 0.5 Mn 1.5 O 4 (LNMO)-based LIBs. Following a detailed comparison of the electrochemical performances of various alkali-metal phosphates, KH 2 PO 4 and NaH 2 PO 4 were selected for an in-depth investigation in this research. The highly protective passivation film generated by KH 2 PO 4 and NaH 2 PO 4 on the electrode surface provided significant protection by effectively inhibiting continuous electrolyte decomposition. This finding was supported by density functional theory calculations and a variety of electrochemical and characterization tests. The H 2 PO 4 − primarily contributed to the formation of the cathode electrolyte interphase film on the cathode surface. KH 2 PO 4 (via the electrostatic shielding effect of K + ions) and NaH 2 PO 4 (through the co-precipitation of Na + and Li + ions) both effectively inhibited the growth of lithium dendrites on the lithium metal anode. Additionally, the KH 2 PO 4 and NaH 2 PO 4 additives regulated the amount of HF in the electrolyte through acid–base equilibrium reactions. The electrolytes containing additives significantly enhanced the electrochemical performances of Li||Li, LNMO/Li, LNMO/graphite, and LNMO/Li 4 Ti 5 O 12 cells. LNMO/Li half-cells with standard electrolyte (STD) supplemented with KH 2 PO 4 and NaH 2 PO 4 additives demonstrated capacity retentions of 92.9 % and 90.0 % after 500 cycles at 5 C, respectively, in contrast to only 79.4 % for the STD electrolyte alone. Furthermore, the LNMO/graphite full cell exhibited an increased capacity retention, reaching 81.1 % (STD+KH 2 PO 4 ) and 78.29 % (STD+NaH 2 PO 4 ), up from 70.8 % with the STD, after 100 cycles at 0.5 C. Given their ease of use, affordability, and widespread availability, KH 2 PO 4 and NaH 2 PO 4 additives show significant potential to enhance the electrochemical properties of high-voltage LIBs.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2025
·Vol. 15
·期 1
·1-14
·
IF 3.9
Wei Aijia,Yang Yuqi,Mu Jinping,He Rui,Li Xiaohui,Zhang Haipeng,Liu Zhenfa,Wang Shasha,Zheng Yong,Mei Shuxing
The instability of the electrode/electrolyte interface and the metal-ions dissolution of high-voltage LiNi 0.5 Mn 1.5 O 4 (LNMO) material lead to significant degradation of cycling performance, thereby limiting the large-scale application of LNMO-based batteries. Here, inorganic Mg/Ca/Sr-contained phosphates (MgHPO 4 , CaHPO 4 , and SrHPO 4 ) are used individually as functional additives of standard electrolytes to enhance the cycling performance of LNMO. Combined with theoretical calculations, a series of electrochemical measurements and characteristics corroborate that the MgHPO 4 is the optimal additive and can preferentially undergo oxidation and reduction decomposition over carbonate solvents. Electrochemical results reveal that the LNMO/Li half-cell containing the MgHPO 4 additive shows a capacity retention of 91.9% after 500 cycles at 5 C, higher than that obtained with STD (76.5%). In addition, the LNMO/graphite (Gr) full-cell with MgHPO 4 additive increases the capacity retention from 70.8 to 78.0% after 100 cycles at 0.5 C. The addition of MgHPO 4 allows a thin, uniform, and conductive cathode-electrolyte interphase (CEI) and solid-electrolyte interphase (SEI) film to be formed on the LNMO cathode and graphite anodes. Furthermore, the preferential reduction of MgHPO 4 inhibits the lithium dendritic growth and enables the formation of a more stable SEI on the Li anode. Besides, the MgHPO 4 additive serves as a scavenger of detrimental HF, thus suppressing the Ni/Mn ions dissolution and improving the structural stability of LNMO. This study provides a cost-effective strategy involving the use of an inorganic additive for improving the electrochemical performance of high-voltage lithium-ion batteries.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Qingtian Li,Tao Wang,Baiyu Guo,Xin Qiao,Xing Meng,Di Jin,Hailong Qiu
As a conversion-type cathode material, FeS 2 emerges as a promising candidate for the next generation of energy storage solutions, attributed to its cost-effectiveness, environment-friendliness and high theoretical capacity. However, several challenges hinder its practical application, including sluggish kinetics, insulating reaction products and significant volume fluctuation during cycling, which collectively compromise its rate capability and cycle stability. Herein, a well-designed sandwich structure of FeS 2 embedded between graphite layers (FeS 2 /C) is obtained using a chloride intercalation and sulfidation strategy. The layered graphite-FeS 2 -graphite configuration boosts the active sites and adsorption capacity of Li + , thereby guaranteeing a high reversible capacity. Furthermore, the graphitic carbon matrix serves a dual purpose: it enhances electronic conductivity and restrain the volume fluctuation of FeS 2 during long cycling. This combination ensures robust electrochemical kinetics, structural integrity and long life. Consequently, the FeS 2 /C composites exhibit exceptional lithium storage performance, achieving capacities of 506.2 mAh g −1 at 0.5 A/g and 277.2 mAh g −1 at 5.0 A/g. Additionally, the FeS 2 /C composites show promising potential as cathodes for all solid-state lithium batteries, showcasing high specific capacities of 658.0 mAh g −1 at 0.1 A/g for the second cycle and maintaining a cycle performance of 288.5 mAh g −1 after 800 cycles at 0.5 A/g. These values surpass the second discharge specific capacity of 96.1 mAh g −1 and cycle capacity of 25.3 mAh g −1 observed for Fe 2 O 3 /C composites. The discharge mechanism of FeS 2 /C composites was further characterized through in-situ transmission electron microscope test. This work provides valuable insights for designing and synthesizing FeS 2 , highlighting its potential for lithium ion storage and all solid-state lithium batteries.
研究领域:
材料科学
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能源存储
✓ 已验证
DOI
高影响因子
IONICS
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2025
·
IF 2.6
Yang Yue,Zhang Zheng,Ma Tianhui,Jia Shaoting,Huang Chao
To achieve high density and high Li-ion conductivity in the garnet LLZO (Li 7 La 3 Zr 2 O 12 ), an effective strategy is to dope it with high-valence elements to stabilize the cubic phase and to lower the sintering temperature. As well known, flash sintering (FS) is characterized by short sintering times and low furnace temperature. Herein, the doping modification of Ta-LLZO by flash sintering at 700 °C for the higher conductivity of LLZO was investigated in the present study. The results indicate that the addition of an appropriate amount of Ta 5+ can enhance the ionic conductivity. The relative density of the sintered cubic Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 is 94.72%, with a corresponding total ion conductivity of 9.8 × 10 –4 S cm −1 , demonstrating good electrical performance. A solid-state lithium metal battery with Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 electrolyte was assembled, and its electrical performance was tested at 50 °C. The results showed that an initial discharge specific capacity of 126.5 mAh g −1 at a 0.1C rate could be reached.
研究领域:
材料科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
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2023
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IF 11.1
Guorong Hu,Kun Huang,Ke Du,Zhongdong Peng,Yanbing Cao
The recovery and regeneration of FePO 4 from lithium extraction slag (LES) are crucial steps in the closed-loop recycling of waste LiFePO 4 batteries . This necessity arises despite the low commercial value of LES, as conventional recovery methods are cost-prohibitive, leading to insufficient attention to LES recovery. The recent surge in retired batteries has resulted in a significant accumulation of LES, posing serious environmental concerns, however, the high content of Fe and P resources in LES presents a potential value. The study begins with a theoretical analysis, concluding that the reduction leaching of LES is a feasible approach. By integrating this with the Fe powder synthesis route for FePO 4 , it is found that efficient leaching of LES can be achieved using a low concentration of H 2 SO 4 , thereby significantly reducing the recovery cost. This method not only efficiently utilize LES but also alleviates environmental pressure. The thermodynamic analysis sheds light on the mechanism of LES leaching and FePO 4 synthesis, confirming the feasibility of each reaction. Optimal leaching conditions (1.4 times the stoichiometric amount of H 2 SO 4 , 1.5 times the amount of Fe powder, an L/S ratio of 5 mL/g, and a reaction duration of 150 min at 60 °C), under which the leaching rates of Fe and P reached 94.66% and 98.23%, respectively. Additionally, the study introduces a method to remove the main impurity Al in LES, achieving a removal rate of over 99%, reducing its concentration to below 100 ppm. Other impurities, such as Ti, Mn, and Zn, also meet the Chinese Chemical Industry Standard (HG/T 4701-2021). Comparative analyses were conducted between regenerated R-FePO 4 , commercial C–FePO 4 , and untreated LES (r-FePO 4 ). LiFePO 4 materials derived from these sources were synthesized, followed by an evaluation of their electrochemical performance. The regenerated R-FePO 4 matched the quality of commercial FePO 4 and significantly outperformed r-FePO 4 . Additionally, the process proposed in this study yields significant economic benefits, estimating a profit of 719.6 $/t of recycled LES. This research proposes a cost-effective and efficient method for regenerating high-quality battery-grade FePO 4 from LES, offering a significant contribution to the closed-loop recycling of waste LiFePO 4 batteries.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
WASTE MANAGEMENT
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2025
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IF 7.1
Yuxue Zhang,Zhaoyong Liu,Jiahui Wang,Hui Du,Qi Sun,Ruitong Gao,Zhenming Xu
Recycling Li from spent lithium ion batteries (SLIBs) in an efficient and highly selective manner could protect the environment and introduce the circular economy principle to society. Simultaneously, the urgent need to address plastic waste, particularly polyvinyl chloride (PVC), has become a global concern. In this work, a strategy for Li extraction through synergetic pyrolysis of LiMn 2 O 4 cathode materials (LMO) and PVC is proposed. Under optimal conditions, the recovery rates of lithium and manganese reached 99.89 % and 0.02 %, respectively, demonstrating efficient separation of these elements. Temperature was found to play a critical role in the leaching rates of lithium and manganese by promoting the decomposition and reduction of LMO. Additionally, kinetic analysis shows that the activation energy ( E a ) of the synergetic pyrolysis is 139.60 KJ/mol, and the pyrolysis mechanism satisfies third-order reaction process. Eventually, the proposed mechanism involves the synergistic effects of chlorination and reduction reactions. First, HCl is generated by PVC pyrolysis under the catalytic effect of LMO. Then, the chlorination of HCl with LMO occurs by capturing structural oxygen and generating LiCl and MnCl 2 . Simultaneously, the reduction reaction between the reducing species generated by PVC pyrolysis and LMO occurs to form Li 2 O and MnO, ultimately enabling the separation of lithium and manganese. Overall, this paper presents a novel approach for future applications by providing a theoretical basis for selective Li extraction.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）