Materials Today Energy
·
2025
·
IF 8.6
Kangwen He,Chi Chen,Shuangjia Weng,Xing Xu,Zhoule Gu,Hongqiao Li,Yang Xia,Yinfeng Wang,Hailing Peng,Xiaoxiao Lu
Ultra-high Ni quaternary cathodes (LiNi x Co y Mn z Al 1-x-y-z O 2 , 1 x 0.8) demonstrate superior cycling stability, positioning them as promising Ni-rich cathode candidates for next-generation lithium-ion batteries. However, increasing demand for higher energy density necessitates higher operation potential, which in turn exacerbates intrinsic challenges, such as poor chemical stability and diminished thermal stability. To address these challenges, an yttrium (Y) modification strategy has been carried out to enhance structural and interfacial stability. Compared to pristine, Y-modified samples show enhanced high-potential and high-temperature performances. In detail, it reveals a specific capacity of 228.5 mAh g −1 within an extended potential window of 3.0–4.5 V and retains 90.7% of its capacity after 200 cycles. When operated at an elevated temperature of 55 °C, it also presents a good capacity retention of 80.4%. The role of Y dopant has been systematically investigated using advanced techniques such as density functional theory (DFT) and in-situ experiments. Results indicate that Y primarily substitutes Ni sites, thereby stabilizing the oxygen framework to enhance cycling stability at a higher operation potential or elevated temperature. Moreover, the formation of surface-coated solid electrolyte layers effectively suppresses interfacial side reactions, contributing to improved cyclability under high-potential and high-temperature conditions.
研究领域:
材料科学
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电化学
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储能技术
·
纳米技术
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无机化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Lianshan Ni,Hongyi Chen,Jinqiang Gao,Yu Mei,Haoji Wang,Wentao Deng,Guoqiang Zou,Hongshuai Hou,Xiaobo Ji
Further popularization of ultrahigh-Ni layered cathodes for high-energy lithium-ion batteries (LIBs) is hampered by their grievous structural and interfacial degeneration upon cycling. Herein, by leveraging the strong electronegativity and low solubility properties of Sb element, a multifunctional modification that couples atomic/microstructural reconstruction with interfacial shielding is well designed to improve the LiNi0.94Co0.04Al0.02O2 (NCA) cathode by combining Sb5+ doping and Li7SbO6 coating. Notably, a robust O framework is established by regulating local O coordination owing to the incorporation of a strong Sb–O covalence bond, leading to the inhibited lattice O evolution at high voltage, as revealed by synchrotron X-ray absorption spectroscopy. Moreover, the radially aligned primary particles with (003) crystallographic texture and refined/elongated sizes are achieved by the pinning of Sb on grain boundaries and are confirmed by scanning transmission electron microscopy, resulting in the fast Li+ diffusion and mitigated particle cracking. Additionally, in situ construction of the Li7SbO6 ionic conductive layer on grain boundaries can effectively boost interfacial stability and Li+ kinetics. As a result, the optimal Sb-modified NCA delivers a high capacity retention of 94.6% after 200 cycles at 1 C and a good rate capacity of 183.9 mAh g–1 at 10 C, which is expected to be applied to next-generation advanced LIBs.
研究领域:
材料科学
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电化学
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储能
·
电池技术
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 35
·期 11
·2209483
·
IF 32.086
Lifan Wang,Guicheng Liu,Rui Wang,Xindong Wang,Liguang Wang,Zhenpeng Yao,Chun Zhan,Jun Lu
Ultrahigh-Ni layered oxides are proposed as promising cathodes to fulfill the range demand of electric vehicles; yet, they are still haunted by compromised cyclability and thermal robustness. State-of-the-art surface coating has been applied to solve the instability via blocking the physical contact between the electrolyte and the highly active Ni 4+ ions on the cathode surface, but it falls short in handling the chemo–physical mobility of the oxidized lattice oxygen ions in the cathode. Herein, a direct regulation strategy is proposed to accommodate the highly active anionic redox within the solid phase. By leveraging the stable oxygen vacancies/interstitials in a lithium and oxygen dual-ion conductor (layered perovskite La 4 NiLiO 8 ) coating layer, the reactivity of the surface lattice oxygen ion is dramatically restrained. As a result, the oxygen release from the lattice is suppressed, as well as the undesired irreversible phase transition and intergranular mechanical cracking. Meanwhile, the introduced dual-ion conductor can also facilitate lithium-ion diffusion kinetics and electronic conductivity on the particle surface. This work demonstrates that accommodating the anionic redox chemistry by dual-ion conductors is an effective strategy for capacity versus stability juggling of the high-energy cathodes.
研究领域:
材料科学
·
电化学
·
储能
·
锂离子电池
·
正极材料
✓ 已验证
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Yuqing Dai,Jiaxu Tan,Zihan Hou,Bianzheng You,Gui Luo,Duo Deng,Wenjie Peng,Zhixing Wang,Huajun Guo,Xinhai Li,Guochun Yan,Hui Duan,Ying Wang,Feixiang Wu,Jiexi Wang
The matching of poly(ethylene oxide) (PEO)-based electrolytes with ultrahigh-nickel cathode materials is crucial for designing new-generation high-energy-density solid-state lithium metal batteries (SLMBs), but it is limited by serious interfacial side reactions between PEO and ultrahigh-nickel materials. Here, a high-concentration electrolyte (HCE) interface with a customized Li+ solvation sheath is constructed between the cathode and the electrolyte. It induces the formation of an anion-regulated robust cathode/electrolyte interface (CEI), reduces the unstable free-state solvent, and finally achieves the compatibility of PEO-based electrolytes with ultrahigh-nickel cathode materials. Meanwhile, the corrosion of the Al current collector caused by lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) ions is prevented by lithium difluoro(oxalato)borate (LiDFOB) ions. The synergistic effect of the double lithium salt is achieved by a well-tailored ratio of TFSI– and DFOB– in the first solvation sheath of Li+. Compared with reported PEO-based SLMBs matched with ultrahigh-nickel (Ni ≥ 90%) cathodes, the SLMB in this work delivers a high discharge specific capacity of 216.4 mAh g–1 (0.1C) even at room temperature. This work points out a direction to optimize the cathode/electrolyte interface.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Nature Energy
·
2024
·Vol. 9
·期 3
·345-356
·
IF 49.7
Zhao Chen,Wang Chuanwei,Liu Xiang,Hwang Inhui,Li Tianyi,Zhou Xinwei,Diao Jiecheng,Deng Junjing,Qin Yan,Yang Zhenzhen,Wang Guanyi,Xu Wenqian,Sun Chengjun,Wu Longlong,Cha Wonsuk,Robinson Ian,Harder Ross,Jiang Yi,Bicer Tekin,Li Jun-Tao,Lu Wenquan,Li Luxi,Liu Yuzi,Sun Shi-Gang,Xu Gui-Liang,Amine Khalil
Surface reconstruction and the associated severe strain propagation have long been reported as the major cause of cathode failure during fast charging and long-term cycling. Despite tremendous attempts, no known strategies can simultaneously address the electro-chemomechanical instability without sacrificing energy and power density. Here we report an epitaxial entropy-assisted coating strategy for ultrahigh-Ni LiNi x Co y Mn 1− x − y O 2 ( x ≥ 0.9) cathodes via an oriented attachment-driven reaction between Wadsley–Roth phase-based oxides and the layered-oxide cathodes. The high anti-cracking and anti-corrosion tolerances as well as the fast ionic transport of the entropy-assisted surface effectively improved the fast charging/discharging capability, wide temperature tolerance and thermal stability of the ultrahigh-Ni cathodes. Comprehensive analysis from the primary and secondary particle level to the electrode level using multi-scale in situ synchrotron X-ray probes reveals greatly reduced lattice dislocations, anisotropic lattice strain and oxygen release as well as improved bulk/local structural stability, even when charging beyond the threshold state of charge (75%) of layered cathodes.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）