LANGMUIR
·
2024
·
IF 3.7
Yue Leng,Shengde Dong,Zhan Chen,Yanxia Sun,Qi Xu,Luxiang Ma,Xin He,Chunxi Hai,Yuan Zhou
In this study, we addressed the poor cycling and rate performance of LiNiO2, a material with ultrahigh nickel content considered a strong contender for high-energy-density lithium-ion battery cathodes. We introduced nano-Al2O3 during the lithiation process to achieve dual modified material through bulk phase element doping and in situ LiAlO2 coating. Comparison revealed notable improvements in the modified materials. In particular, LiNi0.99Al0.01O2 maintained a capacity retention rate of 73.1% after 300 cycles in a long-cycle test at 0.5C current density, outperforming the undoped material. In rate performance tests, the doped samples consistently exhibited higher discharge-specific capacities than that of the undoped counterpart. Notably, at a high current density of 5C, LiNi0.99Al0.01O2 exhibited a discharge-specific capacity of 101.75 mAh g–1. The results indicate that an appropriate amount of Al doping can effectively stabilize the layered structure of the cathode material and delay the irreversible phase transition from H2 to H3. Further, Al doping facilitates the formation of a LiAlO2 coating on the surface of the particles. This coating acts as a fast-ion conductor, enhancing the transport of lithium ions and reducing the erosion of the active material by the electrolyte.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wei-Chen Zheng,Jin-Xia Lin,Hui Chen,Shi-Shi Liu,Chen-Guang Shi,Ling Huang,Shi-Gang Sun
Ni-rich layered oxides are considered ideal positive electrode materials for next-generation state-of-the-art Li-based batteries owing to their high energy densities. However, the structural degradation of Ni-rich positive electrodes and electrolyte decomposition presents significant challenges, particularly at high cut-off voltages. Herein, we report a novel electrolyte consisting of fluorinated solvents that enables the long lifespan of a Li||LiNiO 2 cell with a cut-off voltage of up to 4.5 V. The Li||LiNiO 2 cell retains 93.8% of its initial capacity after 200 cycles. The cycling stability was ascribed to the fluorinated solvents dominating the first structural shell of Li + and deriving a robust cathode-electrolyte interphase (CEI) on the positive electrode. Compared to commercial electrolytes, the fluorinated electrolyte inhibits the structural degradation, stress corrosion cracking, and interphase side reactions of the LiNiO 2 electrode. On the Li negative electrode side, ideal Li plating/stripping and the inhibition of the attack of Ni 2+ are achieved. Furthermore, the 4.5 V-Li||LiNiO 2 cell exhibited a capacity retention of 80.2% after 100 cycles, even under extremely fast-charging conditions.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yue Leng,Shengde Dong,Yanxia Sun,Chunxi Hai,Qi Xu,Yuan Zhou
In this study, high-temperature solid-phase techniques are used to prepare pristine and Mg-modified LiNiO 2 cathode materials. Various characterizations are performed to analyze the morphology, structure, and electrical state of the two materials. Electrochemical tests show that Mg doping effectively improves the electrochemical properties of the materials. In particular, the modified sample exhibits a higher specific discharge capacity of 244.5 mA h g −1 than the pristine sample. Moreover, its maximum capacity retention after 304 cycles at 1 C is 54.1%. In situ X-ray powder diffraction imaging reveals that the modified material has better phase-transition reversibility than the pristine material. Density functional theory calculations indicate that Mg-doped Li sites can accelerate Li + transport. Atomic force microscopy results demonstrate that Mg-doped Li sites act as supportive skeletons that enhance the mechanical properties of the material. Therefore, the proposed strategy for the Mg doping of Li sites can improve the architecture of LiNiO 2 cathode materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Tao Xu,Fanghui Du,Ling Wu,Zhongxu Fan,Lina Shen,Junwei Zheng
The urgent demands of developing Co-free materials for lithium ion batteries with high energy density for next generation electric vehicles have driven the attention of researches to LiNiO 2 stabilized by doping of common elements. Among those elements, manganese is usually used to stabilize cathode material crystal structures to achieve better electrochemical performances. However, the Li + /Ni 2+ cation disorder causing by Mn doping is greatly neglected of the effect on electrochemical behaviors. In order to elucidate the exact effect of Mn-doping, herein, we synthesize Mn-doped LiNiO 2 with extra low Mn content by using the solid-state element thermal interdiffusion strategy. Under calcination at high temperature, with the spherical species coated with Mn-containing gel as the precursor, Mn can be evenly doped into the framework of LiNiO 2 material. It is demonstrated that the small amount of Mn-doping can greatly stabilize both the crystal structure of LiNiO 2 and integrity of the secondary particles during the electrochemical cycling to provide the excellent electrochemical cycling performance and thermal stability of the materials. Nevertheless, the rate capability of the materials is strongly dependent on the amount of the doped Mn, due to the Li + /Ni 2+ cation mixing formed in the synthesis process and introduced in the electrochemical cycling. In the presence of a tiny quantity of the doped Mn, the enlarged crystal lattice would be favorable to the diffusion of the Li + ions in the crystal. However, serious Li + /Ni 2+ cation mixing of the materials with high content of the Mn-doping deteriorates the rate performance of the materials. Thus, in this case, the Mn content is optimized to be 4 mol%, endowing the material with an initial capacity of 202 mAh g −1 at 0.1 C, and a capacity retention of 85.41% after 200 cycles at 0.5 C. For the Mn-doped LiNiO 2 materials, it is suggested that to control the Li + /Ni 2+ cation mixing would be crucial for gaining the materials with superior electrochemical performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2019
·Vol. 3
·期 11
·3234-3243
·
IF 4.912
Shiyi Deng,Yunjiao Li,Qiongyu Dai,Jiamin Fu,Yongxiang Chen,Junchao Zheng,Tongxing Lei,Jia Guo,Jing Gao,Wei Li
The elevation of energy density is the constant pursuit of the lithium-ion battery industry. LiNiO2 has reacquired recognition because it exhibits high capacity without an increase in the cut-off voltages. To address the flaws of this kind of cathodes, herein, trace nano-TiO2-modified LiNiO2 was synthesized via a simple solid-state method. Via combined characterization, the Ti element was verified to be doped into the bulk lattice and located at the transition-metal sites; after Ti doping, the Ni2+ content was clearly increased due to charge balance, followed by an increase in the Li/Ni disorder. The doped Ti and the as-generated Ni pillar mutually facilitated the stabilization of the material structure and benefitted the Li+ de/insertion. Nanosized TiO2 participating in the calcination process could effectively homogenize the size of the primary particles, adjust the surface morphology and reduce the specific surface area of the material. This morphological regulation may be favorable for reducing the contact area of the cathode with the electrolyte and establishing a stable electrode/electrolyte interface, where some detrimental side-reactions take place. With respect to electrochemical properties, Ti doping could decrease the electrode polarization, lower the impedance and promote the Li+ transfer. As a result, the Ti-modified LiNiO2 cathodes, especially the 0.2% Ti-doped (Ti-2) material, presented enhanced electrochemical performances.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 19
·e202300607
·
IF 8.4
Jinmei Wu,Jianwen Yang,Jiawei Zheng,Mengwen Wang,Shengxian Li,Bin Huang,Yanwei Li,Qing Zhu,Quanqi Chen,Shunhua Xiao,Botian Liu
Graphical Co - doping modification of LiNiO 2 : The replacement of Ni atoms with Al 3+ and Ti 4+ ions respectively can improve the charge/discharge cycling performance of LiNiO 2 cathode materials, and their co-doping can more efficiently suppress the Ni 2+ /Li + cation mixing, irreversible phase transition of H2 and H3. Thus, the electrochemical performances exhibit significant synergistic effects. LiNiO 2 cathode material for lithium-ion batteries has the advantages of high specific capacity, abundant resources, and low cost, but it suffers from difficulties in preparation, structural instability, and serious capacity decay. In this work, highly pure and layered structural LiNi 0.95 Al a Ti 0.05- a O 2 ( a =0, 0.025, 0.05) cathode materials were synthesized by a simply sol-gel method. The cation mixing of Ni 2+ and Li + , structural deterioration, irreversible conversion between H2 and H3 phases and unstable surface and CEI (Cathode-electrolyte interface) film can be effectively suppressed by co-doping with Al 3+ and Ti 4+ . A preferred LiNi 0.95 Al 0.025 Ti 0.025 O 2 sample provides a discharge specific capacity of 223 mAh g −1 at 0.1 C and 148.32 mAh g −1 at 5 C, a capacity retention of 72.7 % after 300 cycles at 1 C and a Li + diffusion coefficient of about 2.0×10 −9 cm 2 s −1 .
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-14
·
IF 16.6
Huang Haoliang,Chang Yu-Chung,Huang Yu-Cheng,Li Lili,Komarek Alexander C.,Tjeng Liu Hao,Orikasa Yuki,Pao Chih-Wen,Chan Ting-Shan,Chen Jin-Ming,Haw Shu-Chih,Zhou Jing,Wang Yifeng,Lin Hong-Ji,Chen Chien-Te,Dong Chung-Li,Kuo Chang-Yang,Wang Jian-Qiang,Hu Zhiwei,Zhang Linjuan
Designing efficient catalyst for the oxygen evolution reaction (OER) is of importance for energy conversion devices. The anionic redox allows formation of O-O bonds and offers higher OER activity than the conventional metal sites. Here, we successfully prepare LiNiO 2 with a dominant 3 d 8 L configuration ( L is a hole at O 2 p ) under high oxygen pressure, and achieve a double ligand holes 3 d 8 L 2 under OER since one electron removal occurs at O 2 p orbitals for Ni III oxides. LiNiO 2 exhibits super-efficient OER activity among LiMO 2 , R MO 3 (M = transition metal, R = rare earth) and other unary 3d catalysts. Multiple in situ/operando spectroscopies reveal Ni III →Ni IV transition together with Li-removal during OER. Our theory indicates that Ni IV (3 d 8 L 2 ) leads to direct O-O coupling between lattice oxygen and *O intermediates accelerating the OER activity. These findings highlight a new way to design the lattice oxygen redox with enough ligand holes created in OER process.
研究领域:
材料科学
·
电化学
·
催化
·
能源转换
✓ 已验证
DOI
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Bulletin
·
2026
·
IF 20.7
Yucen Yan,Bianzheng You,Jiping Sun,Zhixing Wang,Guochun Yan,Huajun Guo,Xinhai Li,Wenjie Peng,Gui Luo,Guangchao Li,Bichao Wu,Xing Ou,Junchao Zheng,Feixiang Wu,Hui Duan,Jiexi Wang
The practical application of LiNiO 2 (LNO) is hindered by structural failures such as microcrack propagation and rock-salt phase accumulation, caused by its high reactivity. This study proposes an oxygen vacancy-driven (OVD) strategy, constructing a coherent interface with a Li-containing Ti-doped rock-salt phase on the surface of LNO particles, while introducing a uniform mixed coating layer of TiO 2 and carbon. Unlike electrochemically inert NiO phase, this Li-containing Ti-doped rock-salt phase exhibits high electronic and ionic conductivities, alleviating the anisotropic stress accumulation and suppressing further rock-salt phase formation during cycling. The TiO 2 coating reduces parasitic side reactions at the cathode-electrolyte interface, while the carbon coating further enhances electron transport. As such, OVD-LNO demonstrates exceptional cycling and rate properties, achieving capacity retention of 83.0% after 400 cycles at 1 C and maintaining 188.3 mAh g −1 at 5 C. This pre-constructed rock-salt phase interface modification strategy opens a new pathway for developing high-capacity, long-life cathodes.
✓ 已验证
DOI
PubMed
高影响因子
Progress in Natural Science-Materials International
·
2023
·
IF 4.7
Bianzheng You,Zhixing Wang,Ding Wang,Gui Luo,Duo Deng,Guochun Yan,Huajun Guo,Xinhai Li,Wenjie Peng,Mingxia Dong,Jiexi Wang
LiNiO 2 (LNO) is recognized as the most promising cathode material for next-generation lithium-ion batteries owing to its highest energy density and economic benefit in the layered oxide cathode materials systems. However, severe cation disordering, multiple phase transformations and poor lithium-ion diffusion kinetics , which result in rapid degradation of cycling stabilities and rate properties, hinder its further practical applications. Cobalt doping is an effective strategy to address such issues, but the influences of cobalt on LNO materials have not been figured out completely yet. Hence, a systematical investigation of cobalt doping for LiNiO 2 cathode materials prepared by spray pyrolysis is conducted. The addition of cobalt enhances the stabilities of layered structures and suppresses the cation disordering effectively. The multiple-phase transformations during cycling are also alleviated significantly. Furthermore, cobalt doping can decrease charge transfer resistances and improve lithium-ion diffusion kinetics, especially at high de-lithiation states. As a result, the electrochemical performances are improved comprehensively after cobalt doping. The LNO with optimal doping amount exhibits an improved capacity retention of 78.0% after 100 cycles as compared with 64.9% for pristine LNO, and an outstanding rate performance of 167.2 mA h g −1 with the current density of 5 C (1 C = 200 mA g −1 ).
研究领域:
材料科学
·
电化学
·
能源存储
·
无机化学
·
固态化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Junkai Zhao,Zhixing Wang,Huajun Guo,Xinhai Li
LiNiO 2 -based layered oxides are of great importance as cathode materials for rechargeable batteries. In this paper, illustrating LiNi 0.8 Co 0.15 Al 0.05 O 2 as an example, the effect of nanoscale MnCO 3 treatment on LiNiO 2 -based materials is investigated for the first time. The structures of materials and the properties about the object surface are characterized by XRD, SEM, TEM, EDAX and XPS. The results demonstrate that a part of MnCO 3 is able to react with lithium impurities to form nonstoichiometric Li x Mn y O 4 and the rest of MnCO 3 is converted to MnO 2 coating on the surface of the material in situ. After 100 repeated cycles at 1C, the modified material exhibits a capacity retention rate of 91.2%, while the bare material only remains 84.8%. And the modified material exhibits more significantly improved cycling stability when cycling at 60 °C, maintaining 85.7% of its initial capacity at 1C after 100th cycles. The consumption of Li impurities can decelerate the decomposition of electrolyte during cycling, thus result in less resistive byproducts. Moreover, the obtained MnO 2 coating layer acts as an isolating layer to suppress the drastic reaction between active material and electrolyte. This synergistic effect is responsible for the excellent properties of MnCO 3 -modified material.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Powder Materials
·
2024
·
IF 28.6
Junjie Wang,Yucen Yan,Zilan Zhao,Jiayi Li,Gui Luo,Duo Deng,Wenjie Peng,Mingxia Dong,Zhixing Wang,Guochun Yan,Huajun Guo,Hui Duan,Lingjun Li,Shihao Feng,Xing Ou,Junchao Zheng,Jiexi Wang
LiNiO 2 (LNO) is one of the most promising cathode materials for lithium-ion batteries. Tungsten element in enhancing the stability of LNO has been researched extensively. However, the understanding of the specific doping process and existing form of W are still not perfect. This study proposes a lithium-induced grain boundary phase W doping mechanism. The results demonstrate that the introduced W atoms first react with the lithium source to generate a Li–W–O phase at the grain boundary of primary particles. With the increase of lithium ratio, W atoms gradually diffuse from the grain boundary phase to the interior layered structure to achieve W doping. The feasibility of grain boundary phase doping is verified by first principles calculation. Furthermore, it is found that the Li 2 WO 4 grain boundary phase is an excellent lithium ion conductor, which can protect the cathode surface and improve the rate performance. The doped W can alleviate the harmful H2↔H3 phase transition, thereby inhibiting the generation of microcracks, and improving the electrochemical performance. Consequently, the 0.3 wt% W-doped sample provides a significant improved capacity retention of 88.5 % compared with the pristine LNO (80.7 %) after 100 cycles at 2.8–4.3 V under 1C.
研究领域:
材料科学
·
电化学
·
能源存储
·
无机化学
·
固体物理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）