CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xue Ye,Jianneng Liang,Jiangtao Hu,Dazhuan Wu,Yongliang Li,Xiaoping Ouyang,Qianling Zhang,Xiangzhong Ren,Jianhong Liu
To achieve safe and high energy density solid-state batteries (SSBs), the weight of solid-state electrolyte (SSE) should be minimized and a high voltage and high specific capacity cathode should be used. Polyethylene oxide (PEO)-based polymer electrolytes (PEs) has been identified as the optimal SSE for SSBs owing to their versatile advantages. However, fabricating ultra-thin and high voltage stable PEO-based PEs is still challenging. Herein, an ultra-thin (8.1 µm) blending polymer electrolyte (BPE) is designed through blending PEO, Polymethyl methacrylate (PMMA) and Poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP), and complexing with Succinonitrile (SN), Fluoroethylene carbonate (FEC) and LiTFSI plasticizers. Based on this design, Li|BPE|LiFePO 4 quasi-solid-state battery (QSSB) can operate for 250 cycles with a capacity retention of 92.8%, 4.5 V high voltage Li|BPE|LiCoO 2 QSSB exhibits 87% capacity retention after 80 cycles, with an average Coulombic efficiency ≥99.8%, which is much superior than 4.5 V Li|PEO|LiCoO 2 SSB, whose capacity rapidly decays to 0 mAh/g after a dezen of cycles. DFT calculation suggests that blending PEO, PMMA and PVDF-HFP increase the electrochemical oxidation tolerance. Interface study by TEM and XPS discloses PEO-LiTFSI/LiCoO 2 interface is unstable with a big amount of decomposed products from PEO-LiTFSI and from LiCoO 2 , while BPE/LiCoO 2 interface is more stable without obvious decomposition, indicating the promising application of BPE for high energy density QSSBs.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Zhaoxi Chen,Gaige Zhang,Huayue Yang,Yun Zhao,An Pei,Peng Wang,Jin Yang,Junxi Zhang,Peilin Sun,Haohang Qin,Junzheng Zhan,Jian Peng,Wei-Hsiang Huang,Linan Zhou,Guangxu Chen
The electrochemical upcycling of polyethylene terephthalate (PET) into high-value products is essential for tackling “white pollution” and enhancing environmental protection. However, significant challenges remain, including the need for low-cost, highly efficient electrocatalysts, and the expensive electrolyte recovery in alkaline systems. This study presents a simple doping method to produce Ni octahedral-doped Co3O4 electrocatalysts (NiCo2O4) from spent LiCoO2 (SLCO), enabling sustainable PET upcycling to formic acid (FA) under economic conditions. The NiCo2O4 catalyst exhibits outstanding electrocatalytic activity for the ethylene glycol oxidation reaction (EGOR), achieving a Faradaic efficiency of 90.5% for FA at a potential of 1.50 V versus RHE. When integrated into an anion-exchange membrane (AEM) reactor, the system displayed an average current density of 173.5 mA/cm2 and a Faradaic efficiency of 84.7% at a cell voltage of 1.70 V. Systematic characterizations and DFT calculations indicate that Ni doping alters the spin-state electron density of Co, increases the localized electrons around Co sites, and significantly reduces the charge transfer resistance (Rct from 44.10 Ω to 10.23 Ω) of EGOR. Moreover, the Co–Ni dual sites enhance EG adsorption compared to individual Co or Ni sites. Finally, along with our electrochemical recovery and separation system (ERSS), a KOH recovery rate of 98.9% is achieved, yielding a return of $440.50 per ton of recycled PET─approximately a 4-fold profit increase compared to the traditional acid–base neutralization process (ABNP). This work describes a closed-loop model that simultaneously addresses battery recycling, plastic pollution reduction, and eco-friendly chemical production.
研究领域:
电化学
·
催化
·
环境科学
·
材料科学
·
化学工程
·
废物回收
·
绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Carbon Energy
·
2024
·
IF 19.5
Qihang Ding,Zewen Jiang,Kean Chen,Hui Li,Jingzhe Shi,Xinping Ai,Dingguo Xia
High-voltage LiCoO 2 (LCO) can deliver a high capacity and therefore significantly boost the energy density of Li-ion batteries (LIBs). However, its cyclability is still a major problem in terms of commercial applications. Herein, we propose a simple but effective method to greatly improve the high-voltage cyclability of an LCO cathode by constructing a surface LiF modification layer via pyrolysis of the lithiated polyvinylidene fluoride (Li-PVDF) coating under air atmosphere. Benefitting from the good film-forming and strong adhesion ability of Li-PVDF, the thus-obtained LiF layer is uniform, dense, and conformal; therefore, it is capable of acting as a barrier layer to effectively protect the LCO surface from direct exposure to the electrolyte, thus suppressing the interfacial side reactions and surface structure deterioration. Consequently, the high-voltage stability of the LCO electrode is significantly enhanced. Under a high charge cutoff voltage of 4.6 V, the LiF-modified LCO (LiF@LCO) cathode demonstrates a high capacity of 201 mA h g −1 at 0.1 C and a stable cycling performance at 0.5 C with 80.5% capacity retention after 700 cycles, outperforming the vast majority of high-voltage LCO cathodes reported so far.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Materials Today Nano
·
2022
·
IF 13.364
Q. Sun,X. Chen,J. Xie,C. Huang,X. Xu,J. Tu,C. Shen,Y. Jin,K. Zhang,F. Chen,T. Zhu,X. Zhao,J. Cheng
Garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) ceramics has been considered as an ideal solid-state electrolyte for Li metal cells because of its high ionic conductivity and relatively stable interface with Li. However, it is electrochemically incompatible with some high-voltage cathodes, e.g. LiCoO 2 . In this work, a nanoscale Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) fast ion conductor was coated on LiCoO 2 (only 1 wt% LATP), bringing obviously enhanced interfacial compatibility with a composite electrolyte composed of Al, Nb-codoped LLZO and polyethylene oxide (PEO). A free-standing, flexible and ultrathin (20 μm) electrolyte membrane was successfully fabricated by a facile and scalable route, even though with a high ceramics content (67 wt%). Quasi-solid-state coin and pouch-type Li cells were assembled with the LATP-coated LiCoO 2 cathode, free-standing composite electrolyte and Li anode, together with soft interface modification by in-situ polymerization. The cells show stable cycling due to combined factors of enhanced electrode/electrolyte compatibility, ultrathin nature of the electrolyte membrane and the in-situ built soft interface. The pouch cells can be cycled for 300 cycles at 0.3 C and 60 °C with 80% retention. The pouch cells can endure abuse tests of bending, cutting and nail penetration. At a practical LiCoO 2 loading of 3 mAh cm −2 , the Li|LiCoO 2 pouch cell still shows stable cycling with 90% retention after 100 cycles at 60 °C (0.2 C charge/0.5 C discharge). This work provides a practical method to fabricate high-performance solid-state Li cells.
研究领域:
材料科学
·
电化学
·
固态电池
·
能源材料
·
界面工程
·
纳米技术
✓ 已验证
DOI
高影响因子
Advanced Composites and Hybrid Materials
·
2025
·Vol. 8
·期 4
·286
·
IF 21.8
Mao Gaoqiang,Lu Jingfan,Cai Haiyan,Yu Wanjing,Tong Hui,Guo Xueyi,Zeng Leiying,Jiang Long
Increasing the operating voltage can significantly increase the energy density of LiCoO 2 , but it is accompanied by severe structural damage and interface degradation. Especially at a high voltage above 4.5 V, LiCoO 2 faces severe challenges, such as irreversible phase transition, lattice oxygen loss, and electrode–electrolyte interface evolution. Herein, a high-voltage LiCoO 2 cathode material with bulk doping and surface coating synergistic modification was designed and prepared. The doped Mg 2+ ions entered the lithium layers as pillars, stabilizing the layered framework. Meanwhile, Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 was uniformly coated on the surface of LiCoO 2 , which is beneficial for suppressing Co 3+/2+ ion leaching and interface side reactions during cycling. Furthermore, Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 is a fast ion conductor, which facilitates the rapid transport of lithium ions on the surface of the cathode material. Owing to the synergistic effect of Mg 2+ ion doping and Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 coating, the orbitals of Co 3d and O 2p in LiCoO 2 crystal are changed, and the irreversible phase transition and oxygen loss are inhibited. The modified material exhibited an excellent electrochemical performance. A discharge capacity of 175.5 mAh·g −1 at 10 C rate, as well as a capacity retention of 90.14% after 200 cycles at 1 C rate, was achieved in the modified material. This work supplies a new method for developing high-voltage oxide cathodes through bulk and interfacial modification.
研究领域:
材料科学
·
电化学
·
储能技术
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锂离子电池
·
正极材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Yang Chen,Shujian Liu,Shaokai Cheng,Shuyu Gao,Jingchao Chai,Qiuyue Jiang,Zhihong Liu,Xueqing Liu,Jiyan Liu,Ming Xie,Wubin Dai
The polyvinylidene fluoride (PVdF) binder is the classic binder for cathodes because of its excellent electrochemical stability and superior adhesion property. However, PVdF is very expensive and sensitive to moisture. Therefore, pursuit of a cost-effective binder is highly desirable, especially for high-voltage cathode application. Polyacrylonitrile (PAN) possesses strong polar C≡N groups, endowing it with oxidation resistance and strong binding properties. Herein, the PAN binder was systematically investigated for the electrochemical performance of the 4.5 V high-voltage LiCoO2 (HV-LCO) electrode. The results showed that the HV-LCO-PAN electrode delivered superior rate capability and cycling stability to the corresponding HV-LCO-PVdF. The PAN binder was highly tolerant of moisture and was capable of forming uniform coating on the cathode materials. Moreover, the PAN binder had ultrahigh mechanical modulus (8.01 GPa) and hardness (381.45 MPa) in a liquid electrolyte, thereby improving cycling stability and rate capability. X-ray photoelectron spectroscopy analysis further demonstrated that PAN formed uniform coating on the surface of LiCoO2 and played a role of an artificial cathode–electrolyte interphase layer, suppressing decomposition of the liquid electrolyte under high cutoff voltage.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Wei Feng,Jianling Li,Huirong Liu,Mingliang Zhao,Jianjian Zhong,Jiameng Feng
Poly(ethylene oxide) based polymer electrolytes(PEO-SPEs) suffer from a narrow electrochemical window and deliver poor electrochemical performance when coupling with 4.2 V cathode. This severely limits the scope of its application. Here, a combination of physical stirring and electrochemistry is used to form an ultrathin and uniform cladding layer on the LiCoO 2 particles. The results show that in addition to the decomposition of LiPO 2 F 2 during the charge/discharge cycling, decomposition reactions occur during the stirring and drying process by X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscope (FESEM) and transmission electron microscope (TEM). This novel method effectively improves the electrochemical performance of 4.2 V PEO based solid-state lithium batteries . In particular, the cell shows excellent and stable electrochemical performance, exhibiting a discharge capacity of 112.0 mAh g −1 after 200 cycles, a capacity retention rate of 79.4% and a capacity decay rate of approximately 0.1% per cycle when the surface of LiCoO 2 is coated with 2 wt% LiPO 2 F 2 . In comparison, the discharge capacity of the unmodified LiCoO 2 cathode is found to be only 75.6 mAh g −1 after 100 cycles, with a poor capacity retention rate of 56.8%. Based on the basis of the above research, a new process was explored and also shows excellent interfacial stability by dispersing LiPO 2 F 2 directly inside the binder which with a discharge capacity of 109.2 mAh g −1 and a capacity retention rate of 84.5% after 145 cycles. This novel approach opens up a new pathway for solving the problem of interfacial stability between PEO based polymer electrolytes and high-voltage cathode.
研究领域:
材料科学
·
电化学
·
固态电池
·
聚合物电解质
·
能源存储
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Lixiong Bai,Wendong Xue,Haixia Qin,Yan Li,Yong Li,Jialin Sun
A dense LiCoO 2 microcrystalline buffer layer for an all-solid-state lithium battery is designed and prepared as a stable interface using a magnetron sputtering method. The LiCoO 2 microcrystalline buffer layer possesses a large interfacial specific surface area and excellent interfacial stability. The interfacial contact resistance of the modified interface is reduced by 1279 Ω compared to the unmodified interface. The mode of the structure of the modified interface is established by material studio, and the potential energy barrier is calculated by ab initio theory based on the structure model. The results show that the barrier to the migration of interfacial Li ion is only 0.097 eV, which is only 1/5 of that in the grain interior. The electrochemical performance is measured by using a cathode with a slurry mixture composed of LiNi 0.5 Co 0.2 Mn 0.3 O 2 and polymer electrolyte . The results show that the electrochemical properties of the all-solid-state lithium batteries are significantly improved by the addition of the LiCoO 2 microcrystalline layer, with the battery showing an initial discharge capacity of 149.5 mAh g −1 and a discharge capacity of 121.2 mAh g −1 after 50 cycles at 0.1 C and 60 °C.
研究领域:
材料科学
·
电化学
·
电池技术
·
固态电解质
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Ruoxuan Qi,Ming Yang,Tianle Zheng,Xingchen Liu,Yonggao Xia,Ya-Jun Cheng,Peter Müller-Buschbaum
The LiCoO 2 (LCO) cathode is foreseen for extensive commercial applications owing to its high specific capacity and stability. Therefore, there is considerable interest in further enhancing its specific capacity by increasing the charging voltage. However, single-crystal LCO suffers from a significant capacity degradation when charged to 4.5 V due to the irreversible phase transition and unstable structure. Herein, an ultra-small amount (0.5% wt. in the electrode) of multi-functional PIM-1 (a polymer with intrinsic microporosity) additive is utilized to prepare a kind of binder-free electrode. PIM-1 modulates the solvation structure of LiPF 6 due to its unique structure, which helps to form a stable, robust, and inorganic-rich cathod-eelectrolyte interphase (CEI) film on the surface of LCO at a high voltage of 4.5 V. This reduces the irreversible phase transition of LCO, thereby enhancing the cyclic stability and improving the rate performance, providing new perspectives for the electrodes fabrication and improving LCO-based high-energy-density cathodes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
EXTREMOPHILES
·
2022
·Vol. 26
·期 2
·1-16
·
IF 3.035
Liu Dehong,Shi Hongjie,Chen Guanglin,Zhang Xu,Gu Tingyue,Zhu Minglong,Tan Wensong
High metal ion concentrations and low pH cause severely inhibit the activity of an acidophilic microbial consortium (AMC) in bioleaching. This work investigated the effects of exogenous spermine on biofilm formation and the bioleaching efficiency of LiCoO 2 by AMC in 9K medium. After the addition of 1 mM spermine, the activities of glutathione peroxidase and catalase increased, while the amount of H 2 O 2 , intracellular reactive oxygen species (ROS) and malondialdehyde in AMC decreased. These results indicated that the ability of AMC biofilm to resist oxidative stress introduced by 3.5 g/L Li + and 30.1 g/L Co 2+ was improved by spermine. The activity of glutamate decarboxylase was promoted to restore the intracellular pH buffering ability of AMC. Electrochemical measurements showed that the oxidation rate of pyrite was increased by exogenous spermine. As a result, high bioleaching efficiencies of 97.1% for Li + and 96.1% for Co 2+ from a 5.0% (w v −1 ) lithium cobalt oxide powder slurry were achieved. This work demonstrated that Tafel polarization can be used to monitor the AMC biofilm’s ability of uptaking electrons from pyrite during bioleaching. The corrosion current density increased with 1 mM spermine, indicating enhanced electron uptake by the biofilm from pyrite.
研究领域:
环境科学
·
微生物学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Guisheng Zeng,Chongwen Hu,Rui Zhou,Juyong Wang,Xianfu Liu,Jianwen Huang,Jiaping Yu,Guanghui Wu,Zhongbing Wang,Chunjian Deng,Junwei He,Chunli Liu,Xubiao Luo
With the impending increase in the number of retired lithium-ion batteries, effective recycling and upcycling strategies must be explored to alleviate resource shortages, address environmental pollution, and meet the growing demand for high-performance cathode materials. This study proposes a closed-loop upcycling strategy that utilizes current collector aluminum (Al) as both a dopant and raw material for surface coating. This approach repairs the structural defects of highly degraded LiCoO 2 (LCO) cathode materials and achieves bulk Al doping and surface LiAlO 2 coating, transforming them into high-performance cathode materials capable of stable operation at a high voltage of 4.5 V. Specifically, bulk Al doping suppresses irreversible phase transitions and enhances structural stability, while the LiAlO 2 coating improves interfacial charge transfer and mitigates polarization. The synergistic effects of these modifications collectively enhance the electrochemical stability of LCO. The upcycled material delivers an initial discharge capacity exceeding 181.5 mAh g -1 and retains 93.9% of its capacity after 200 cycles at 1 C. Even under a high current rate of 10 C, the discharge capacity remains above 150.1 mAh g -1 , thereby outperforming commercial LCO cathodes. This study provides a simple and efficient solution for the direct upcycling of degraded LCO cathode materials into high-performance alternatives.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 33
·期 8
·2212869
·
IF 19.924
Jing Xia,Na Zhang,Yijun Yang,Xing Chen,Xi Wang,Feng Pan,Jiannian Yao
Cycling lithium cobalt oxide (LiCoO 2 ) to a potential higher than 4.35 V (vs Li + /Li) can obtain an enticing capacity, but suffers from inferior structural stability. Herein, an ingenious Li-deintercalation/doping strategy is developed to synthesize the lanthanide-doped LiCoO 2 (lanthanide (Ln) = praseodymium, neodymium, samarium, europium, gadolinium, erbium, or lutetium) with Ln occupying Li-sites. Electrochemical measurements show that the cycling stability of Ln-doped LiCoO 2 increases as the lanthanide contracts. By rule, lutetium-doped LiCoO 2 exhibits the best cycling stability, confirmed in both lithium half-cell and pouch full-cell. Comprehensive experimental characterizations combining with theoretical calculations reveal that the lattice strain tuned by the lanthanide contraction plays a critical role in the structure stability of LiCoO 2 . This finding is an important step for building better high-voltage LiCoO 2 batteries, as it is possible to achieve better high-voltage performance by combining the doping technology and performance improvement rule disclosed in this study.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）