CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jingsheng Xu,Zhiyuan Wang,Runguo Zheng,Hongyu Sun,Yanguo Liu,Junhua You
Ni-rich cathodes especially with Ni content over 90 % are promising next-generation cathode materials for advanced high energy lithium − ion batteries. However, in comparison with Ni ≤ 80 % Ni-rich cathodes, these ultrahigh Ni-rich materials face more severe challenges in terms of harmful H2 − H3 phase transformations and structural degradation during cycling. Herein, we present a robust surface structure composted of defect-rich disordered structures and LiF/Li 2 SiO 3 coating for stabilizing the ultrahigh Ni-rich cathode LiNi 0.96 Co 0.03 Mn 0.01 O 2 (NCM96) by modification with (NH 4 ) 2 SiF 6 . The surface disordered structures including Li/TM mixing, spinel, and rock salt structure play a crucial role in inhibiting the irreversible H2-H3 phase transition and reducing lattice volume changes by lattice coherence effect. Moreover, the disordered surface in collaboration with the co-coating restrains the rapid growth of surface rock salt phase into the bulk, enhancing structural stability. The modified sample NSF-0.5 delivers a capacity of 238 mAh/g at 0.1C and maintains a capacity retention of 88.5 % at 0.5C after 100 cycles in half cell as well as 82.3 % at 1C after 300 cycles in full cell, significantly superior to the NCM96. The findings provide a simple and cost-effective surface modification strategy to enhance the structural stability and electrochemical performance of ultrahigh nickel cathodes for high-energy density LIBs.
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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锂离子电池
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固态化学
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表面工程
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电池材料
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
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2025
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IF 5.6
Chen Liu,Siwu Li,Lin Li,Qiyue Luo,Liang Ming,Ziling Jiang,Ziyu Lu,Miao Deng,Jie Yang,Shijie Cheng,Chuang Yu
The sulfide electrolyte-based all-solid-state batteries with high-nickel layered oxide cathodes face significant challenges due to the narrow electrochemical window of sulfides and severe side reactions caused by direct contact with high-voltage oxide cathode materials such as LiNi 0.9 Mn 0.05 Co 0.05 O 2 (NCM90). Here, we successfully synthesized Li 3 InCl 6 (LIC) halide electrolytes through ball-milling followed by annealing method, achieving the ionic conductivity of 2.0 mS cm −1 at room-temperature. The interface between this electrolyte and NCM90 cathode material without any interface modification is stable. By introducing the LIC electrolyte layer, the NCM90/LIC+Cl1.5/Li-In battery exhibits significantly improved electrochemical performance at different temperatures, particularly in terms of initial discharge capacity. Notably, the battery demonstrates outstanding discharge capacity and cycling stability at low temperatures. Experimental investigations reveal that the introduction of the LIC electrolyte with high oxidation potential facilitates the H2-H3 phase transition in NCM90 during high-voltage operation, which is critical for enhancing the discharge capacity. This work provides fundamental insights into interfacial engineering strategies for high-voltage sulfide-based all-solid-state battery systems.
研究领域:
储能
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材料科学
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电化学
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固态电池技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Maosheng Gong,Yadong Wei,Hongzhou Zhang,Jingyuan Liu,Xin Zhang,Xuanming Chang,Peiyu Hou,Xijin Xu,Lianqi Zhang
High-capacity Ni-rich cathodes hold considerable promise in advancing both high-energy Li-ion batteries (LIBs) and all-solid-state Li batteries (ASSLBs). Yet, lattice volume changes induced by the H2–H3 phase transition lead to structural degradation. It has been demonstrated that doping approaches can enhance structural stability. Nevertheless, the selection of an appropriate dopant is of considerable importance for the design of high-performance Ni-rich materials with high-entropy doping. Furthermore, the feasibility of high-entropy doped Ni-rich cathodes in ASSLBs has not been reported to date. In this study, leveraging the chemically competitive doping mechanism of Mg, Al, Ti, Nb, and Mo elements, we propose a high-entropy doped LiNi0.8Co0.1Mn0.05Mg0.01Al0.01Ti0.01Nb0.01Mo0.01O2 (HE-NCM) to stabilize Ni-rich cathodes. In-situ X-ray diffraction confirms that the synergistic effect of multiple dopants in high-entropy doping significantly alleviates the H2–H3 phase transition and reduces lattice volume changes, which contribute to the absence of microcracks and improved bulk/interface stability. In ASSLBs, the HE-NCM@LiNbO3 maintains an outstanding capacity retention of 84.5% even after 1700 cycles, demonstrating the feasibility of high-entropy doped Ni-rich cathodes when matched with a sulfide solid-state electrolyte. The application of high-entropy doping methodology for the development of advanced rechargeable batteries has been shown to provide a novel perspective on the improvement of the structural robustness and interfacial compatibility of Ni-rich cathode materials.
研究领域:
材料科学
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电化学
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储能技术
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锂离子电池
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固态电池
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
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2025
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IF 17.1
Yujing Wu,Ziqi Zhang,Dengxu Wu,Fuqiang Xu,Mu Zhou,Hong Li,Liquan Chen,Fan Wu
Sulfide solid-state electrolytes (SEs), prized for high ionic conductivity and mechanical strength, face practical challenges due to multi-field coupling failures under operational stresses. While prior studies emphasize electrochemical degradation (e.g., interfacial reactions, Li dendrites), thermal failure mechanisms during high-temperature storage remain overlooked. This work systematically explores calendar aging in sulfide-based all-solid-state batteries (ASSBs). Among tested systems, LiCoO₂ (LCO), Li 6 PS 5 Cl, and Li-In alloy exhibit superior stability after high-temperature storage. However, high-voltage LiNi 0.8 Co 0.1 Mn 0.1 O₂ (NCM811) undergoes structural collapse, releasing decomposition products that accelerate interfacial reactions and thermal failure. Batteries at high states of charge (SOC) experience intensified self-discharge-driven electrode-electrolyte reactions at elevated temperatures. In contrast, LCO-Li 6 PS 5 Cl-LiIn ASSBs at 0 SOC retain nearly undegraded performance after 5 days at 90°C. Suppressing the detrimental H3-phase transition in NCM811 improves capacity retention by ≥21%. The study elucidates high-temperature degradation pathways in sulfide ASSBs, linking thermo-electro-chemical coupling effects to interfacial ion transport barriers and contact degradation. These insights advance the understanding of calendar aging mechanisms, providing critical guidance for predicting battery lifespan and designing robust electrode/electrolyte systems.
研究领域:
材料科学
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电化学
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储能
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电池技术
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热稳定性
✓ 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）