Nanoscale
·
2021
·Vol. 13
·期 16
·7822-7830
·
IF 7.79
Yuwan Dong,Panzhe Su,Guanjie He,Huiling Zhao,Ying Bai
With high theoretical capacity and tap density, LiCoO2 (LCO) cathode has been extensively utilized in lithium-ion batteries (LIBs) for energy storage devices. However, the bottleneck of structural and interfacial instabilities upon cycling severely restricts its practical application at high cut-off voltage. From another perspective, the compatibility between the electrode and electrolyte is highly valued in the development of all-solid-state batteries. Herein, we construct a compatible interface between Li7La3Zr2O12 (LLZO) and LCO through a facile surface modification strategy, which significantly improves the cycling stability of LCO at a high cut-off voltage of 4.5 V. Characterization results demonstrate that the LCO@1.0 LLZO sample delivers a desirable capacity retention of 76.8% even after 1000 cycles at 3.0–4.5 V with the current density of 1 C (1 C = 274 mA g−1). Further investigation indicates that the LLZO modification layer could protect the LCO electrode through effectively alleviating the side reactions, which not only facilitates the Li+ transportation at the interface but also mitigates the bulk structure degradation. Moreover, it is also established that a small amount of La and Zr ions could gradiently migrate into the surface lattice of LCO to generate a thin layer of the surface solid solution Li–Co–La–Zr–O. Thus formed pinning region between surface modified LLZO and LCO cathode could contribute both to their mechanical compatibility and Li+ kinetics behavior upon repeated cycling. This work not only provides a strategy in broadening the operation potential and extracting higher capacity of LCO but also sheds light on constructing compatible interfaces in LIBs, especially for all-solid-state energy storage and conversion devices.
研究领域:
材料科学
·
能源存储与转换
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DOI
PubMed
高影响因子
ChemSusChem
·
2025
·Vol. 18
·期 15
·e202500148
·
IF 6.6
Chong Ni,Xuyong Feng,Yuanyun Dou,Wentao Wu,Hongfa Xiang
Surface coating is an efficient way to reduce side reactions between cathode materials and electrolytes, thus enhancing the cycle stability of cathode materials. In this study, a novel surface-coating strategy based on the melt curing process is introduced, which forms an ionic conductive LiAlO 2 layer on the surface of LiCoO 2 /LiNi 0.5 Mn 1.5 O 4 cathode materials and enhances the cycle stability of these cathode materials. Comprehensive characterizations, including scanning electron microscopy, energy dispersive spectrometer, and transmission electron microscopy (TEM) confirm the uniformity and thin LiAlO 2 coating. Electrochemical performance tests show better cycle performance of LiCoO 2 with 1% LiAlO 2 coating. An 85% capacity can be retained over 200 cycles at 1C and 4.5 V cutoff, compared to 61% for uncoated LiCoO 2 . For LiNi 0.5 Mn 1.5 O 4 , the coated sample shows 94.5% capacity retention after 300 cycles at 1C, while the capacity of the uncoated sample decays to 64.6% under the same condition. These findings underscore the effectiveness and universality of this surface-coating strategy. Graphical In this study, a novel surface-coating strategy based on a melt curing process is proposed, which forms an ion-conductive LiAlO 2 coating layer on the surface of LiCoO 2 cathode materials. TEM combined with EDS, XPS, etc. confirms the uniform thin layer LiAlO 2 coating, while the electrochemistry measurements prove the high stability of LiCoO 2 with LiAlO 2 coating.
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yu Peng,Jiawei Chen,Gaopan Liu,Yue Yin,Xiaoli Fang,Yonggang Wang,Xiaoli Dong,Yongyao Xia
Lithium metal batteries (LMBs) with Li metal anodes and high-voltage LiCoO 2 (LCO) cathodes offer high energy density but face challenges such as Li dendrite growth and LCO structure degradation, which primarily arises from the electrolyte's inability to form a stable interphase. Herein, a dual-additive optimized carbonate-based electrolyte is developed, incorporating tetraethylammonium nitrate (TEANO 3 ) and lithium difluorobis(oxalato) phosphate (LiDFBOP) as regulators. LiDFBOP enhances interfacial stability and compactness, while TEANO 3 facilitates Li + transport and suppresses excessive decomposition of LiDFBOP. The synergistic effect of TEANO 3 and LiDFBOP establishes robust, high ion-conductive solid electrolyte interphase (SEI) and cathode–electrolyte interphase (CEI) enriched with P- and N-containing inorganic compounds (including LiN x O y and P-O/P-F species), enabling dense Li deposition and stable cycling of LCO under a high cut-off voltage of 4.5 V. The optimized electrolyte enables Li||LCO full cells with a high capacity retention of 84% even with high-mass-loading LCO cathode (3.5 mAh cm −2 ) and limited Li (N/P = 2). This work demonstrates a straightforward electrolyte design strategy for optimizing SEI and CEI, advancing the practical deployment of LMBs.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Journal of Energy Storage
·
2021
·
IF 6.583
Weikang Zheng,Zongyang Li,Guang Han,Qiannan Zhao,Guanjie Lu,Xiaolin Hu,Jing Sun,Ronghua Wang,Chaohe Xu
Lithium-ion capacitors (LICs) have become one of the most popular energy storage devices because of the combination of high energy densities and power densities. However, the kinetic imbalance of anode and cathode restricts the specific capacities and voltage windows of LICs. Herein, an in-situ nitrogen-doped activated porous carbon (ANMPC) material with high specific surface area (1894.9 m 2 /g) is proposed to act as both cathode and anode for the preparation of the 4.5 V “all carbon” LICs. The hierarchically porous ANMPC obtained by KOH activation and carbonization of polypyrrole (PPy) has plenty of mesopores created by surfactant (added during the PPy process) as well as micropores generated by KOH activation, thus can provide abundant active sites for ion intercalation and large area for electrostatic adsorption simultaneously, satisfying the critical requirements of high-performance anode and cathode, respectively. After coupling the pre-lithiated ANMPC anode and fresh ANMPC cathode, the complete LIC device delivers large energy density of 167.5 Wh/kg at a power density of 269.0 W/kg, and still remains 88.9 Wh/kg at an ultrahigh power density of 13,198.5 W/kg, exhibiting enormous potential for applications in high performance lithium-ion capacitors.
研究领域:
材料科学
·
能源存储技术
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Binbin Chu,Longzhen You,Guangxin Li,Tao Huang,Aishui Yu
More and more attention has been focused on Ni-rich ternary materials due to their superior specific capacity, but they still suffer inherent structural irreversibility and rapid capacity degradation under a high voltage. Oxidation of unstable oxygen will lead to the irreversible transformation of the structure. Taking into account the strong W–O bond, an appropriate amount of W-doping is studied to reinforce the thermal stability and electrochemical performance of LiNi0.6Co0.2Mn0.2O2 (NCM622) at 4.5 V. Combining experiments and theoretical calculations, it can be found that W-doping is most preferred at Co sites, and the average charge around O in the NiO6 octahedron becomes more negative after W-doping, which can successfully restrain the release of oxygen, thereby improving the stability of the crystal structure during deep delithiation. In addition, W-doping decreases the energy barrier of the Li+ migration slightly and boosts the kinetic diffusion of lithium ions. As a result, NCM622 doped with 0.5% W boasts an outstanding capacity retention of 96.7% at 1 C after 100 cycles and a discharge specific capacity of up to 152.8 mA h g–1 at 5 C between 3.0 and 4.5 V. Furthermore, analysis of the cycled electrodes indicates that the lattice expansion and the formation of microcracks during long cycling are suppressed after W-doping, thereby elevating the structure and interface stability. Therefore, doping an appropriate amount of W via simple methods is helpful to obtain Ni-rich cathode materials with admirable performance.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
Nanoscale Research Letters
·
2020
·Vol. 15
·期 1
·1-10
·
IF 3.578
Song Shipai,Peng Xiang,Huang Kai,Zhang Hao,Wu Fang,Xiang Yong,Zhang Xiaokun
The stability issue of LiCoO 2 cycled at high voltages is one of the burning questions for the development of lithium ion batteries with high energy density and long cycling life. Although it is effective to improve the cycling performance of LiCoO 2 via coating individual LiCoO 2 particles with another metal oxides or fluorides, the rate capacity is generally compromised because the typical coating materials are poor conductors. Herein, amorphous Li 0.33 La 0.56 TiO 3 , one of the most successful solid electrolytes, was directly deposited on the surface of made-up LiCoO 2 electrodes through magnetron sputtering. Not only the inherent conductive network in the made-up LiCoO 2 electrodes was retained, but also the Li + transport in bulk and across the cathode-electrolyte interface was enhanced. In addition, the surface chemical analysis of the cycled LiCoO 2 electrodes suggests that most of the stability issues can be addressed via the deposition of amorphous Li 0.33 La 0.56 TiO 3 . With an optimized deposition time, the LiCoO 2 electrodes modified by Li 0.33 La 0.56 TiO 3 performed a steady reversible capacity of 150 mAh/g at 0.2 C with the cutoff voltage from 2.75 to 4.5 V vs . Li + /Li and an 84.6% capacity gain at 5 C comparing with the pristine one.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
eScience
·
2022
·
IF 0
Wei Gu,Guoyong Xue,Qingyu Dong,Ruowei Yi,Yayun Mao,Lei Zheng,Haikuo Zhang,Xiulin Fan,Yanbin Shen,Liwei Chen
Ni-rich layered oxides are attractive cathode materials for advanced lithium-ion batteries (LIBs) due to their high energy density. However, their large-scale application is seriously hindered by their interfacial instability, especially at a high cut-off potential. Here, we demonstrate that trimethoxyboroxine (TMOBX) is an effective film-forming additive to address the interfacial instability of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) material at a high cut-off voltage of 4.5 V. We find that TMOBX decomposes before carbonate solvent and forms a thin cathode electrolyte interphase (CEI) layer on the surface of the NCM811 material. This TMOBX-formed CEI significantly suppresses electrolyte decomposition at a high potential and inhibits the dissolution of transition metals from NCM811 during cycling. In addition, electron-deficient borate compounds coordinate with anions ( P F 6 − , F − , etc.) and H 2 O in the battery, further improving the battery's stability. As a result, adding 1.0 wt% of TMOBX boosts the capacity retention of a Li||NCM811 cell from 68.72% to 86.60% after 200 cycles at 0.5C in the range of 2.8–4.5 V.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Chaowei He,Hangjun Ying,Lucheng Cai,Hengquan Chen,Zuojie Xu,Shenwen Liu,Pengfei Huang,Haiyuan Zhang,Wenlong Song,Jian Zhang,Lu Shi,Weiwei Gao,Dan Li,Wei-Qiang Han
Solid-state lithium metal batteries (SSLMBs) with poly (ethylene oxide) (PEO)-based electrolytes have increasingly become one of the most promising battery technologies due to high energy density and safety. However, adverse electrode/electrolyte interface compatibility issues hinder further application. Herein, a PEO-based composite solid electrolyte with excellent anode and cathode interfacial compatibility is designed via the coordination modulation strategy induced by lithium difluorobis(oxalato)phosphate (DFBOP). By utilizing this electrolyte, the robust inorganic-rich interphase involving LiF, Li x PO y F z , and P─O components is in situ generated on lithium (Li) anode and LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode surfaces via forceful coordination among PEO, lithium bis(trifluoromethanesulphonyl)imide, and DFBOP and subsequent adjustment of front orbital energy levels. It contributes to homogeneous lithium deposition and an effective impediment of PEO oxidation decomposition at high voltage, promoting superior interfacial stability. Consequently, Li-symmetric cells with modified electrolyte can achieve a stable cycle over 7000 h at 0.2 mA cm −2 . Specially, the cathode electrolyte interphase with a unique organic–inorganic interpenetration network structure enables the 4.5 V Li/NCM811 cells to cycle steadily over 100 cycles, with a high discharge capacity of 215.4 mAh g −1 and initial coulombic efficiency of 91.23%. This research has shed light on the interfacial design of PEO-based electrolytes from the perspective of electrolyte coordination regulation to construct high-performance SSLMBs.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Weikang Zheng,Zongyang Li,Guanjie Lu,Tongxin Yang,Menghong Li,Chaohe Xu,Ronghua Wang
Lithium-ion capacitors (LICs) possess high energy density and power density simultaneously. However, for balancing electrochemical performance, mechanical properties and safety issues, the development of high-performance electrodes and electrolytes is still a challenge in this field. Herein, a 3D nitrogen-doped carbonaceous foam (N C) was synthesized by chemical vapor deposition (CVD), and the covering of poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP) dramatically increase its flexibility without decreasing the electrochemical performance. The complete quasi-solid-state LICs using N C/PVDF-HFP as anode, N C/activated carbon (AC)/PVDF-HFP as cathode and PVDF-HFP as the skeleton of gel electrolyte are fabricated and shows good cycle stability (72.2 % after 2000 cycles). Meanwhile, the power density of the LIC can reach up to 342.5 W/kg when the energy density is 209.3 Wh/kg, and the power density can reach as high as 7632.2 W/kg at energy density of 77.6 Wh/kg, which is higher than many other dual-carbon and quasi-solid-state LICs.
研究领域:
材料科学
·
能源存储技术
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2026
·
IF 5.5
Zhi-Qiang Li,Li-Yun Xing,Yi Yang,Xiao-Ke Wang,Yu-Xi Huang,Chong Yan
High-energy-density lithium batteries increasingly operate under high voltage and fast charging, with interfacial stability and reaction kinetics at elevated temperature becoming critical bottlenecks. Conventional electrolytes undergo severe parasitic reactions, leading to transition-metal dissolution, increased interfacial resistance, and rapid capacity fading, which hinder simultaneous stability and rate capability. Here, an electrolyte design combining molecular engineering and interfacial regulation is proposed. An α-H-free ester solvent, methyl 2-fluoro-2-methylpropanoate (MFMP), enhances oxidative stability, while its weak solvation reshapes the Li+ solvation structure and promotes anion participation, forming an inorganic-rich cathode electrolyte interphase (CEI). A functional additive, ethylene sulfate (DTD), further regulates interfacial reactions at elevated temperatures, leading to a more uniform interphase and lower charge-transfer resistance. The electrolyte delivers stable cycling and improved rate performance at 4.5 V and maintains low resistance and stable capacity at 45 °C. Structural analysis reveals suppressed cathode degradation and reduced parasitic reactions. This work establishes a multiscale strategy linking molecular design, solvation, and interfacial chemistry for batteries under extreme conditions.
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DOI
高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 18
·2203999
·
IF 27.8
Lifan Wang,Guicheng Liu,Rui Xu,Xindong Wang,Liguang Wang,Zhenpeng Yao,Chun Zhan,Jun Lu
The Ni-rich layered oxide cathode is pushing the frontier of battery powered electric vehicles toward longer driving range and lower cost, whilst facing a major challenge with the compromised cycle life and thermal robustness. It is well recognized that irreversible oxygen evolution at the cathode-electrolyte interphase is critical to the electrochemical and thermal stability of the Ni-rich cathode. Herein, combining experiments with density functional theory (DFT) calculations, the authors focus on manipulating the irreversible oxygen evolution to solve the performance degradation and safety hazard. An oxygen ion conductor introduced to the surface of the cathode restrains the activated surficial lattice oxygen ions by its stable oxygen vacancies. Meanwhile, a Li-rich fast ion conductor incorporated in the coating layer synergistically reinforces the Li diffusion path through the cathode-electrolyte interphase. This sophisticated multifunctional surficial modification implemented by a neat one-step treatment represents a successful design and development of a thermally stable Ni-rich cathode and approximately 400-cycle state-of-health up to 80% with the operating voltage range extended up to 4.5 V. Therefore, this study provides an encouraging strategy to overcome the capacity versus robustness dilemma of high-energy cathodes.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
固体离子学
·
电池技术
·
表面工程
✓ 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
·
锂离子电池
·
正极材料
✓ 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）