APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
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2025
·Vol. 131
·期 9
·1-11
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IF 2.8
Wang Jiatai,Li Yuanyuan,Fan Chao,Li Jiting,Wen Xi,Liu Hongyun,Zhang Xuchao,Ma Xiaohong,Hu Jingfu,Li Jian
High-nickel LiNi 0.9 Co 0.01 Mn 0.09 O 2 cathode materials demonstrate significant potential for next-generation lithium-ion batteries (LIBs) due to their high energy density and low cost. However, the reduced cobalt content in these high-nickel materials often results in structural degradation and poor cycling stability. In this work, the material referred to as NCM919 was prepared through a homogeneous co-precipitation method, followed by the introduction of W 6+ doping to enhance cycling stability. The electrochemical performance results indicate that the cathode doped with 1.0 mol% W 6+ (NCM-1.0 W) exhibits improved electrochemical characteristics. NCM-1.0 W shows an initial discharge capacity of 182.74 mAh/g at a rate of 0.5 C, with 97.86% of the initial capacity retained after 100 cycles within a voltage range of 2.5 ~ 4.3 V. Additionally, NCM-1.0 W achieves an initial discharge capacity of 197.99 mAh/g at a rate of 1.0 C, with 85.68% of the initial capacity maintained after 100 cycles in a voltage range of 2.5 ~ 4.5 V.
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高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
J. LUO,J.X. Liu,F.M. Xiao,L. Huang,W.C. Li,R.H. Tang,Q. Zhou,Y. Wang
In order to restrain the capacity decay of nickel-rich materials for lithium-ion batteries (LIBs) in advanced energy applications, a Ni-rich cathode (LiNi 0.88 Co 0.07 Al 0.05 O 2 , LANCA) with high-rate capability and cycle life was designed and prepared by coating γ-LiAlO 2 and doping Al 3+ on the surface and inside of the secondary particles, respectively. Specifically, the γ-LiAlO 2 -coated and Al 3+ -doped LANCA samples were synthesized by a simple strategy of pre-coating Ni 0.88 Co 0.07 Al 0.05 (OH) 2 , based on aluminum isopropoxide hydrolysis combined with a post-sintering lithiation process. With the γ-LiAlO 2 and Al 3+ , the capacity retention ratio of the cathode is tremendously improved from 61.7 to 83.6% at 1 C rate after 100 cycles. Even at a heavy current density of 10 C for the LANCA cathode, a high reversible capacity of 154.4 mA h g − 1 can be acquired, which amount to the 82.5% capacity retention at 0.2 C. Detailed morphology and structure observation shows that the side reaction at the electrolyte-cathode interface was suppressed, the structural degradation and intergranular cracking were suppressed, while the diffusion of Li + and conductivity were improved. Therefore, this ingenious structural design has certain reference significance for the development and commercialization of high-performance cathode materials for electric power.
研究领域:
材料科学
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电化学
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能源存储
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无机化学
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固态化学
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DOI
高影响因子
Journal of the American Chemical Society
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2023
·
IF 15
Feng Li,Xiaobin Cheng,Gongxun Lu,Yi-Chen Yin,Ye-Chao Wu,Ruijun Pan,Jin-Da Luo,Fanyang Huang,Li-Zhe Feng,Lei-Lei Lu,Tao Ma,Lirong Zheng,Shuhong Jiao,Ruiguo Cao,Zhi-Pan Liu,Hongmin Zhou,Xinyong Tao,Cheng Shang,Hong-Bin Yao
Solid electrolytes (SEs) are central components that enable high-performance, all-solid-state lithium batteries (ASSLBs). Amorphous SEs hold great potential for ASSLBs because their grain-boundary-free characteristics facilitate intact solid–solid contact and uniform Li-ion conduction for high-performance cathodes. However, amorphous oxide SEs with limited ionic conductivities and glassy sulfide SEs with narrow electrochemical windows cannot sustain high-nickel cathodes. Herein, we report a class of amorphous Li–Ta–Cl-based chloride SEs possessing high Li-ion conductivity (up to 7.16 mS cm–1) and low Young’s modulus (approximately 3 GPa) to enable excellent Li-ion conduction and intact physical contact among rigid components in ASSLBs. We reveal that the amorphous Li–Ta–Cl matrix is composed of LiCl43–, LiCl54–, LiCl65– polyhedra, and TaCl6– octahedra via machine-learning simulation, solid-state 7Li nuclear magnetic resonance, and X-ray absorption analysis. Attractively, our amorphous chloride SEs exhibit excellent compatibility with high-nickel cathodes. We demonstrate that ASSLBs comprising amorphous chloride SEs and high-nickel single-crystal cathodes (LiNi0.88Co0.07Mn0.05O2) exhibit ∼99% capacity retention after 800 cycles at ∼3 C under 1 mA h cm–2 and ∼80% capacity retention after 75 cycles at 0.2 C under a high areal capacity of 5 mA h cm–2. Most importantly, a stable operation of up to 9800 cycles with a capacity retention of ∼77% at a high rate of 3.4 C can be achieved in a freezing environment of −10 °C. Our amorphous chloride SEs will pave the way to realize high-performance high-nickel cathodes for high-energy-density ASSLBs.
研究领域:
材料科学
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电化学
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能源存储
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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
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电化学
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能源存储
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DOI
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Shuai Li,Tianxiang Yang,Wenlian Wang,Jing Lu,Xiaoyang Zhao,Weizhen Fan,Xiaoxi Zuo,Junmin Nan
2-thiophene sulfonamide (2-TS) is demonstrated as a multi-functional additive to functionalize the electrolyte and improve the performances of LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811)/graphite batteries . Compared with the batteries without 2-TS, the performances of batteries with 2-TS containing electrolyte are significantly improved at wide temperature and high cut-off charge voltage of 4.40 V (vs. Li/Li + ）. After 500 cycles at room temperature and in the voltage range of 2.80–4.20 V, the batteries with 1% 2-TS and without 2-TS additive lose 8.40% and 23.59% initial discharge capacity, respectively. At an elevated temperature of 45 °C and in the voltage range of 2.80–4.40 V, the cycle performance of the batteries with 1% 2-TS is also enhanced, i.e., 68.68% initial discharge capacity is remained after 115 cycles, while the batteries without 2-TS has already decayed to the lifespan point. It is shown that 2-TS molecules can both consume the H 2 O/HF residues to alleviate the decomposition of LiPF 6 and preferentially react on the electrodes to form uniform and dense low-resistance films. These results demonstrate this electrolyte can effectively improve the battery performances and has promising prospects applying in high-voltage and high-nickel NCM-based batteries.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Feng Chen,Xinqi Zhu,Weilong Dai,Congcong Yao,Junchao Qian,Zhigang Chen,Chengbao Liu
The high nickel cathode LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 (combination of NCM and NCA) coated with the Li + conductor Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 in various mass fractions was prepared via using the typical sol-gel process. The LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 after the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 covering demonstrated the similar crystal structure and particle morphology in comparison with the bare cathode. The electrochemical test results indicated the superior rate capabilities and cycling performances were acquired for the coated cathodes due to the presence of the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 film on the surface of LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 . The 2 wt% Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 covered LiNi 0.83 Co 0.06 Mn 0.06 Al 0.05 O 2 exhibited the greatest electrochemical performance with a large cycle retention rate of 90.9% over 300 cycles at 45 °C, rate capacity of 139.8 mAh g −1 at 5 C current density, and a high capability of 126.5 mAh g −1 at − 30 °C, superior than those (80.9%, 99.8 mAh g −1 , 71.3mAh g −1 accordingly) of the bare cathode. In addition, the safety and environmental reliability tests of pouch batteries suggested the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 film on the surface of cathode acted as a protective layer to promote the stability for application.
研究领域:
材料科学
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电化学
·
能源存储
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Hua Yan,Yu-hong Luo,Ying Lei,Qing-lin Pan,Jun-chao Zheng
N ickle (Ni)-rich layered oxides as promising candidate of high-capacity cathode materials have aroused extensive concern primarily regarding their higher specific capacity. However, the major hurdle of Ni-rich cathodes (Ni content ≥0.7) is their poor cycling stability, which often suffers from the release of oxygen, structural degradation and increased impedance during cycling, especially at high voltage or high temperature. Herein, we demonstrated a feasible solid phase method for easy industrialization based on the Al 3+ /Zr 4+ co-doping in LiNi 0.72 Co 0.05 Mn 0.23 O 2 (A X Z Y -NCM) single-crystal cathode. The optimized A 0.5 Z 0.5 -NCM single-crystal material exhibited greatly enhanced structural and thermal stability. XRD refinement results indicated that both Al 3+ and Zr 4+ were mainly located in transition metal (TM) sites, strengthening the layered structure through strong M-O bonds and inhibiting cation mixing. In-situ XRD revealed that the synergistic rivet effect of Al/Zr co-doping alleviates anisotropic lattice stress-strain during charge/discharge process. Accordingly, the A 0.5 Z 0.5 -NCM cathode can output a high initial capacity of 177.3 mAh g −1 at 1 C, and captured a more desirable capacity retention of 85.10 % than that of U-NCM (74.33 %) at 1 C over 200 cycles. Even at a high voltage of 4.5 V, its capacity retention can still reach 82.37 %, significantly surpassing the unmodified U-NCM (31.0 %). The above results demonstrated that well-designed dual doping is highly effective for strengthen structure stability and cycling performance of Ni-rich cathodes.
研究领域:
材料科学
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电化学
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能源存储与转换
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高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 36
·期 13
·2311553
·
IF 29.4
Ruyu Shi,Nengzhan Zheng,Haocheng Ji,Mengtian Zhang,Xiao Xiao,Jun Ma,Wen Chen,Junxiong Wang,Hui-Ming Cheng,Guangmin Zhou
Direct regeneration of spent lithium-ion batteries has received wide attention owing to its potential for resource reuse and environmental benefits. The repair effect of direct regeneration methods undergoing heterogeneous repair process is usually inferior, while homogenous repair process plays a vital role to achieve satisfactory repair results. However, the practical applications of current homogeneous repair methods are challenged by the complex operations and relatively high costs owing to the requirement of additional heating or pressurization. Herein, this work proposes a simple strategy to achieve homogeneous repair of spent cathode materials under relatively mild conditions by uniformly precoating lithium source at room temperature and atmospheric pressure. Followed by annealing, highly degraded LiNi 0.83 Co 0.12 Mn 0.05 O 2 with severe Li deficiency and irreversible phase transition is repaired to have an initial capacity of 181.6 mAh g -1 and capacity retention of 80.7% after 150 cycles at 0.5 C. The lithium source used in this strategy is from the spent lithium anode. Moreover, this strategy is suitable for the direct regeneration of various layer oxide cathode materials with different failure degrees. This work provides both theoretical guidance and practical examples for the straightforward, effective, and universally applicable direct regeneration methods.
研究领域:
材料科学
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电化学
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能源存储
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可持续技术
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电池回收
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jingyan Huang,Chong Xu,Jia Wang,Zengjie Fan,Lei Xu,Yu He,Xingyu Zhang,Bing Ding,Xiaogang Zhang
Compared to liquid electrolytes, gel polymer electrolytes (GPEs) offer enhanced safety and represent an up-and-coming option for high-energy–density lithium metal batteries (LMBs). However, several challenges hindered the practical application of GPEs for LMBs, such as low ionic conductivity at room temperature, decomposition at high voltage, and poor interfacial compatibility with lithium anode. In this study, a non-flammable fluorinated GPE was synthesized using 2,2,2-trifluoroethyl acrylate (TFEA) and ethoxylated trimethylolpropane triacrylate (ETPTA) as precursor materials, with succinonitrile (SN) incorporated as a plasticizer and a dual-salt system of lithium bis(trifluoro-methane) sulfonimide and lithium difluoroxalate borate. Notably, the as-prepared GPE exhibits a high ionic conductivity of 1.33 mS cm −1 at 30 °C, an electrochemical stability window of 5.15 V ( vs . Li + /Li), and excellent interfacial compatibility with the high-nickel LiNi 0.93 Co 0.035 Mn 0.035 O 2 (NCM-93) cathode and lithium metal anode. Consequently, the Li|NCM-93 cells demonstrated outstanding cycling stability at a cutoff voltage of 4.3 V at room temperature as well as exceptional safety performances under high-temperature conditions and intense radiation conditions. Furthermore, the fluorinated GPE effectively suppresses the gas generation from high-nickel cathode materials and inhibits the growth of lithium dendrites on the anode. This work offers a novel avenue for developing safe and high-voltage solid-state LMBs for working in harsh environments.
研究领域:
材料科学
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能源存储技术
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DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Zhaowen Bai,Subash Kandasamy,Wei Wang,Rui Zhou,Zhenjie Zhang,Xuefeng Wang,Jiatu Liu,Zhenbin Wang,Guohua Chen,Qingyu Kong,Tianyi Li,Yang Ren
High-nickel layered oxides are promising cathode materials for next-generation lithium-ion batteries due to their high energy density, but their structural instability at high voltages remains a critical challenge. This study investigates how Ni migration influences phase segregation, Li/Ni antisite defect accumulation, and mechanical degradation in LiNiO2 (LNO) through a combination of synchrotron X-ray diffraction (XRD), extended X-ray absorption fine structure (EXAFS), transmission electron microscopy (TEM), and density functional theory (DFT) calculations. The results reveal that at high voltages, Ni migrates into tetrahedral sites, leading to the formation of coexisting R3̅m phases with distinct lattice behaviors. This phase segregation induces inhomogeneous lithium distribution, internal stress, and strain accumulation, ultimately promoting microcrack formation and accelerating structural degradation. While Ni migration is partially reversible upon discharge, continuous cycling leads to the progressive accumulation of Li/Ni antisite defects, which disrupt Li-ion transport and further destabilize the structure. The findings describe the role of bulk Ni migration in phase segregation, linking atomic-scale lattice distortions to long-term performance limitations in high-Ni cathodes. These insights suggest strategies such as selective doping to mitigate Ni migration and improve the structural stability.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xinhong Hu,Kai Du,Yujia Zhang,Yabin Hou,Huiling Zhao,Ying Bai
With high specific energy density, Ni-rich layered LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) material has become one promising cathode candidate for advanced lithium-ion batteries (LIBs). However, severe capacity fading induced by microstructure degradation and deteriorated interfacial Li + transportation upon repeated cycling makes the commercial application of NCM cathode in dilemma. To address these issues, LiAlSiO 4 (LASO), one unique negative thermal expansion (NTE) composite with high ionic conductivity, is utilized as a coating layer to improve the electrochemical performances of NCM material. Various characterizations demonstrate that LASO modification can endow NCM cathode with significantly enhanced long-term cyclability, through reinforcing the reversibility of phase transition and restraining lattice expansion, as well as depressing microcrack generation during repeated delithiation-lithiation processes. The electrochemical results indicate that LASO-modified NCM cathode can deliver an excellent rate capability of 136 mAh g −1 at a high current rate of 10 C (1800 mA g −1 ), larger than that of the pristine cathode (118 mAh g −1 ), especially higher capacity retention of 85.4% concerning the pristine NCM cathode (65.7%) over 500 cycles under 0.2 C. This work provides a feasible strategy to ameliorate the interfacial Li + diffusion and suppress the microstructure degradation of NCM material during long-term cycling, which can effectively promote the practical application of Ni-rich cathode in high-performance LIBs.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Jian Fan,Chunyan Cao,Lan Shang,Liangjie Yuan
High-nickel layered oxide LiNi 0.9 Co 0.1 O 2 is a promising cathode material for lithium-ion batteries due to its high specific capacity and low cost. However, the internal stress generated during deep delithiation can cause microcracks, giving rise to rapid capacity decay and deteriorated thermal stability. In this work, Mg and Al ions are incorporated into the bulk phase of LiNi 0.9 Co 0.1 O 2 via high-temperature solid-state reaction. We demonstrate that Al 3+ doping enhances charge transfer between transition metal (TM) and oxygen layers, strengthening TM-O bonds and stabilizing the structure, thereby alleviating structural distortions under deep delithiation. More impressively, Mg 2+ doping significantly improves structural stability through a pillaring effect, effectively suppressing irreversible phase transitions during charge-discharge cycling. Consequently, Mg-Al co-doping optimizes the overall structural integrity of the high-nickel cathode, enhances its stability, and inhibits lattice oxygen release during long-term cycling. The Mg-Al co-doped LiNi 0.9 Co 0.1 O 2 delivers a remarkable capacity of 177.3 mAh g −1 after 100 cycles with capacity retention of 93.5 %, demonstrating outstanding cyclability. This Mg-Al co-doping strategy provides a simple and practical approach to enhance the electrochemical performance of high-nickel layered cathode materials.
研究领域:
材料科学
·
电化学
·
锂离子电池
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DOI
高影响因子
危险品化学品经营许可证（带存储）