APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yunchao Liao,Na Wang,Xinyi Dai,Wenwen Zhou,Fuzhong Wu,Jiexi Wang,Haijun Chen,Yi Mai
Ultrahigh-nickel LiNi x Co y Mn 1-x-y O 2 cathode material (Ni content ≥ 0.9) is of great significance for the development of high energy density of lithium-ion batteries. However, its high surface activity leads to more surface residual lithium formation and deterioration of electrochemical performance, especially at high voltage. Here we add NH 4 F and nitrogen-doped carbon nanotubes (CNT) during the dimethyl carbonate (DMC) washing process, and constructed in situ the nano-LiF and CNT composite cathode electrolyte interphase (CEI) layer while removing part of residual lithium, effectively optimizing the surface environment of LiNi 0.9 Co 0.05 Mn 0.05 O 2 . The modified LiNi 0.9 Co 0.05 Mn 0.05 O 2 has a capacity retention rate of 61.3 % after 200 cycles between 2.8 and 4.5 V at 1C, significantly higher than the 46.7 % of the unwashed sample, and a specific discharge capacity of 146.9 mAh g −1 at 5C, compared to 127.5 mAh g −1 for the unwashed sample. Benefit from the alleviation of polarization and the increase of Li + diffusion coefficient, the stable CEI layer provides effective protection for LiNi 0.9 Co 0.05 Mn 0.05 O 2 under 4.5 V, alleviating surface side reactions. In this paper, a simple and effective strategy is developed to optimize the surface of Ni-rich cathode material, which provides a new insight for the treatment of surface residual lithium.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2025
·Vol. 41
·期 2
·333-342
·
IF 3
Lin Huahui,Shen Yu,Wei Li,Song Ran,Wu Fan,Wei Peng,Yang Zhenzhong,Ren Yurong,Qu Ke,Ding Zhengping
Ultra-high nickel layered cathodes (Ni⩾95%) have emerged as prospective candidates for next-generation lithium-ion batteries (LIBs) due to their exceptional specific capacity and cost-effectiveness. However, the commercial application of these cathodes has been hindered by several challenges, including structural instability during cycling, high sensitivity to air, and slow Li + migration. In this research, a one-step modification strategy was developed to simultaneously achieve Mg doping and Li 3 PO 4 layer coating for the ultra-high nickel cathodes. Characterization results demonstrated that Mg doping not only alleviates lattice strain changes during the H2–H3 phase transition (H2: the second hexagonal phase; H3: the third hexagonal phase) but also serves as a structural anchor, preventing Ni 2+ migration and occupation within the Li layer. The Li 3 PO 4 surface coating layer acts as an electrochemical shield, protecting against interfacial side reactions and enhancing the Li + diffusion rate. As a result, the LiNi 0.95 Mn 0.05 O 2 cathode, with both internal and external modifications, demonstrates significant improvement in cycling stability (85.7% capacity retention after 100 cycles) and Li + transport performance (130.6 mA·h·g −1 at 10 C, 1 C=189.6 mA·h·g −1 ), providing a solid foundation for the further development and application of ultra-high nickel cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jianlong Wang,Honglin Yan,Cheng Wei,Yuan Ha,Weidong Zhu,Lu Li,Chaoyi Zhou,Qianxin Xiang,Zhimin Li,Yue Hao
Ultra-high Ni layered cathodes LiNi x Mn 1- x O 2 ( x > 0.9) with high energy density for lithium-ion batteries suffer from severe fatigue failure upon cycling because of the unstable crystal structures at highly delithiated states. Despite efforts to address this issue, enhancing the structural stability by electrostatic interaction between oxygen layers has been overlooked. Herein, we propose an electrostatic interaction strategy via Mn-Mg-Al-Ti medium-entropy doping to improve the fatigue resistance of the crystal structure. As expected, these chosen dopants efficiently impede the distortion, interlacement, and fracture of transition metal slabs in crystal structures by enhancing the electrostatic interaction. Accordingly, the cathode LiNi 0.93 Mn 0.04 Mg 0.01 Al 0.01 Ti 0.01 O 2 delivers superior cycling performance with a capacity retention of 96.1 % at 0.5C after 100 cycles. This work demonstrates the effectiveness of improving the electrochemical performance of ultra-high Ni cathodes by the electrostatic interaction strategy, which is of great significance for their commercial application.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2025
·
IF 12.1
Xilong Chen,Zhili Yu,Xiangjie Li,Zhaoyu Sun,Guozheng Ma,Qiyun Li,Yingchun Ou,Yuxuan Liu,Renzong Hu
Ultrahigh-nickel layered oxide cathodes (≥90% nickel) possess exceptionally high discharge capacities, which can significantly improve the energy density of lithium-ion batteries and alleviate the driving range anxiety of electric vehicles. However, the high interfacial reactivity of ultrahigh-nickel cathodes, especially the detrimental side reactions with harmful acidic species like HF in the electrolyte, can deteriorate the battery interface and reduce the cycle life, hindering their practical application. In this study, 3-isocyanatopropyltrimethoxysilane (PTTS-NCO) is introduced as the electrolyte additive, which can effectively scavenge the harmful acidic species in the electrolyte and form a protective surface layer at the electrode/electrolyte interface, thereby enhancing the electrochemical performance of the battery (NCM90/Li). Specifically, the most effective battery based on the PTTS-NCO additive can maintain 70.3% of its capacity after 500 cycles at 30 °C. Even under a high cathode loading (3.0 mAh cm −2 ), it can retain 86.2% of its capacity after 300 cycles, far exceeding the base battery. Furthermore, it exhibits good performance under the harsh high-temperature environment, maintaining over 70.3% capacity retention in the NCM90/Li battery up to 350 cycles at 60 °C. This work demonstrates the great potential of multifunctional siloxane additive in lithium batteries based on ultrahigh-nickel cathode.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yuqing Dai,Zihan Hou,Xin Yu,Zihan Yan,Yiman Feng,Gui Luo,Duo Deng,Wenjie Peng,Zhixing Wang,Huajun Guo,Hui Duan,Xing Ou,Jun-Chao Zheng,Jiexi Wang
Ultrahigh-nickel cathode active materials (CAMs) suffer from detrimental side reactions when coupled with poly(ethylene oxide) (PEO)-based electrolytes in solid-state lithium–metal batteries (SLMBs). To circumvent this issue, here we propose a surface modification strategy for ultrahigh-nickel CAMs with a self-assembled nanoscale polymer coating. Without requiring additional initiators, the residual lithium compounds inherent on the surface of the ultrahigh-nickel CAMs are used as initiators to induce the in situ anionic polymerization of the monomer. Meanwhile, oxygen vacancies are generated on the surface through the coordination of –C = O and –C ≡ N with transition metal ions, which reduces the diffusion barrier for Li+ in their vicinity. Benefiting from the high voltage stability, rapid Li+ transfer, and elasticity of the coating layer, the coated LiNi0.9Co0.06Mn0.04O2 exhibits a capacity retention of 92% after 100 cycles when matched with PEO-based electrolytes. The pouch cell enables stable operation for 500 cycles at 1C. In addition, we propose to measure the MW of recycled PEO after cycling by gel permeation chromatography, which is direct evidence that decomposition (cleavage of the ether linkages) of PEO is inhibited. As a vision, this efficient, high-yield, and simple nanoscale coating method is expected to promote the commercial application of SLMBs.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Zhiwen Wang,Zhenping Qiu,Chaojie Zhao,Zheng Pan,Guangxia Wang,Yue Guo
As demand for high-energy-density batteries grows, cobalt-free ultra-high‑nickel cathodes like LiNiO₂ are poised to revolutionize next-generation energy storage solutions. However, their practical use is hindered by structural degradation caused by phase transitions, oxygen loss, and detrimental interfacial reactions triggered by the strong oxidizing nature of Ni 4+ formed under high voltage, which together lead to rapid capacity degradation and poor cycling stability. To overcome these challenges, effective doping strategies are crucial. This study systematically examines the potential of Mn and Al doping to enhance the stability of LiNiO₂ using in situ XRD, TEM, XPS, and electrochemical testing. The results show that, while both Mn and Al doping enhance structural stability and cycling performance, they operate through different mechanisms. In particular, 4 mol% Al doping remarkably suppresses c-axis expansion, enhances phase transition reversibility, and achieves capacity retention of 84.8 % after 100 cycles at 1C. In contrast, LiNiO₂ exhibits good tolerance toward Mn doping up to 10 mol%, which helps mitigate structural degradation; however, the capacity retention remains moderate at 80.3 %. While Al doping primarily enhances electrochemical performance, Mn doping contributes to preserving the structural integrity of the cathode at higher concentrations. Our study reveals their complementary roles, providing a strategy to address structural challenges and advance sustainable cobalt-free energy storage solutions.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2024
·
IF 9
Bao Zhang,Heng Wen,Keyi Xian,Na Lu,Chao Zheng,Zhiming Xiao,Xinyou He,Long Ye,Jiexi Wang,Lei Ming,Chunhui Wang,Xing Ou
Ultrahigh nickel cobalt-free layered oxide cathode is considered to be one of the most promising lithium-ion cathode materials due to its high specific capacity and low price. Unfortunately, high nickel cathode materials have problems such as high cation mixing, thermal stability and structure instability, and how to address these problems has been the direction of researchers. Introducing heteroatoms into bulk phase is an essential and effective method for dealing with the above issues. In this paper, the comprehensively reinforced crystal and framework structure has been obtained in LiNi 0.9 Mn 0.1 O 2 (NM-WMM) cathode material by the synchronously doping of W 6+ , Mg 2+ and Mo 6+ . Thanks to the pillar function of all the doping elements and robust metal-O bond of W 6+ and Mo 6+ , the structural and chemical stability of the designed materials have been effectively strengthened, contributing to enhance their cycling performance and high-temperature properties, and optimize the reaction kinetics synchronously. As expected, NM-WMM materials deliver a prominent capacity retention rate at both 25 °C (91 %, 200 cycles, 1 C) and 50 °C (93.9 %, 100 cycles, 1 C). This proves that the multi-element doping modification strategy is beneficial to improve the cyclic performance and thermal stability of Ni-rich Co-free cathode materials.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态化学
·
电池技术
✓ 已验证
DOI
高影响因子
Tungsten
·
2025
·
IF 11.2
Zhou Jie,Zhang Yu-Hang,Mao Qin-Zhong,Xu Xing,Reng Zi-Rui,Yao Zhu-Jun,Xia Yang,Lu Xiao-Xiao
Ultra-high Ni layered cathodes are considered leading candidates for next-generation lithium-ion batteries due to their high energy density. However, their practical application is hindered by structural instability, rapid capacity degradation, and sluggish lithium-ion kinetics. To overcome these challenges, a synergistic modification strategy combining gradient Nb doping with in situ formation of a LiNbO 3 surface layer is proposed. The radially distributed Nb dopant effectively mitigates internal lattice strain and suppresses the formation of microcracks, while the LiNbO 3 coating enhances interfacial stability and facilitates Li-ion transport. As a result, the optimized sample (0.5%Nb-NCM) delivers a high specific capacity of 222.2 mAh·g −1 at 0.1C, retains 94.7% of its capacity after 200 cycles at 1C, and achieves 147.7 mAh·g −1 at an ultra-high rate of 20C. This work highlights the effectiveness of combining compositional and interfacial engineering to develop structurally robust and electrochemically stable ultrahigh-Ni cathodes for advanced Li-ion battery applications. Graphical abstract
研究领域:
电化学
·
材料科学
·
能源存储
·
锂离子电池
·
界面工程
·
结构稳定性
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
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
·
电化学
·
能源存储
·
锂离子电池
·
固态化学
·
表面工程
·
电池材料
✓ 已验证
DOI
高影响因子
Chemical Science
·
2024
·Vol. 15
·期 32
·12964-12972
·
IF 7.6
Yuqing Dai,Zihan Hou,Gui Luo,Duo Deng,Wenjie Peng,Zhixing Wang,Huajun Guo,Xinhai Li,Guochun Yan,Hui Duan,Wenchao Zhang,Jiexi Wang
Benefiting from high energy density of ultrahigh-nickel cathode materials and good safety of PEO-based electrolytes, PEO-based ultrahigh-nickel solid-state lithium batteries (SLMBs) are considered to be new-generation energy storage devices. However, the incompatibility of ultrahigh-nickel cathode materials and PEO-based electrolytes is the main challenge due to serious interfacial side reactions. Therefore, the modification of the cathode/electrolyte interface is crucial. Herein, the residual lithium on the surface of LiNi0.9Co0.06Mn0.04O2 is utilized to construct an interfacial coating layer by reacting with H3BO3. The in situ formed xLi2O-B2O3 coating layer (LBO1-NCM) with high ionic conductivity can be regulated with different crystal structures during the sintering process. Besides, an all-solid-state three-electrode cell is fabricated, which verifies that the xLi2O-B2O3 coating can effectively stabilize the interface. Astonishingly, uneven Li anode deposition is observed in SLMBs, which is caused by the breakage of PEO molecular chains due to the strong oxidation of the cathode, while this crosstalk is also suppressed by the xLi2O-B2O3 coating layer. Consequently, Li|PEO|LBO1-NCM achieves a substantially improved electrochemical performance, exhibiting 90.5% of capacity retention after 100 cycles for the coin cell and 80.3% of capacity retention after 200 cycles for the pouch cell. Apparently, the targeted modification of interfaces should be paid as much attention as electrolyte optimization in SLMBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Xiangdong Zhu,Caiyan Shen,Tian Qiu,Yu Zhang,Wei Xu,Guorong Hu,Yanbing Cao,Zhongdong Peng,Ke Du
Driven by the growing demand for energy density of lithium-ion batteries, ultra-nickel- rich layered oxides LiNi x Co y Mn z O 2 (x > 0.9) (ultra-Ni-rich NCM) cathodes attract considerable attention. However, these cathode materials suffer from severe structural degradation during cycling, primarily due to phase transitions, which significantly hinders their long-term application. In this work, ultra-Ni-rich NCM cathode materials with Co- and Mn-rich surface architectures are synthesized using Co/Mn-rich shell precursors and are systematically investigated to evaluate the suitability of different surface chemistries under various electrochemical conditions. The results reveal that the Co-rich surface significantly enhances the electrochemical kinetics by mitigating the Li + concentration gradient between the surface and bulk, thereby effectively suppressing structural degradation. In contrast, the Mn-rich surface, due to the presence of electrochemically inert Mn 4+ , leads to sluggish kinetics and incomplete phase transitions within the voltage window of 2.8–4.3 V. This results in a lower capacity but notably improved structural integrity. Upon increasing the upper cutoff voltage to 4.4V, the Mn-rich shell cathode undergoes more complete phase transitions, leading to a substantial improvement in capacity while maintaining superior structural stability.
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Steven Hu,Xinghui Liang,Huimin Yuan,Zhenning Xu,Jun Wang,Hai Liu,Kaihua Xu,Xing Ou
The development of Co-free ultrahigh-Ni (Ni > 0.9) layered oxide cathode materials holds immense promise for addressing electric vehicle range limitations and cost efficiency, though substantial obstacles persist in structural durability, thermal stability, and safety. To concurrently enhance the structural integrity and interfacial stability of LiNi 0.95 Mn 0.05 O 2 , a dual-functional co-regulation strategy integrating Zr/Al bulk doping with Li 6 Zr 2 O 7 surface coating is implemented. Controlled Zr 4+ /Al 3+ co-incorporation expands interlayer spacing, strengthens transition metal–oxygen bonding, and stabilizes the oxygen framework, thereby improving Li + diffusion kinetics while suppressing cation disorder. Concurrently, the epitaxially Li 6 Zr 2 O 7 coating effectively passivates the surface by eliminating residual lithium species, inhibiting grain coarsening, and suppressing interfacial side reactions. These coupled bulk-surface modifications synergistically inhibit mechanical stress-induced crack propagation and deleterious phase transformations. Therefore, the optimized cathode achieves 96.9% capacity retention after 100 cycles at 1 C, while maintaining stable operation under extreme electrochemical conditions (4.5 V cutoff voltage) and thermal extremes (−10 °C/60 °C). This work demonstrates a synergistic modification paradigm for designing robust ultrahigh-Ni cathodes, thereby propelling the advancement of next-generation high-energy density lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
✓ 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）