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ACS Applied Energy Materials · 2024 · IF 5.4

High Entropy and Co-Free High Nickel Based Layered LiNi0.9Mn0.1O2 Cathode for Li-Ion Batteries

Seokyoung Choi,Wuliang Feng,Yongyao Xia

High nickel and Co-free layered cathodes (LiNi0.9Mn0.1O2, NM) for lithium-ion batteries (LIBs) have gained researchers’ interest recently because of their high energy density and being free of toxic elements, but they still suffer from inferior electrochemical performance due to the lattice instability during cycling. Herein, we successfully improved the electrochemical performance of NM using a high-entropy strategy. A high nickel Co-free multidoped high-entropy LiNi0.9Mn0.05Zr0.01Nb0.01Ti0.01Al0.01Mg0.01O2 (HE-NM, where HE represents high entropy with Zr, Nb, Ti, Al, and Mg dopants) cathode with five dopants was successfully synthesized. Owing to the effect of the multidopant, parasitic reactions and the accumulation of rock-salt phase were successfully suppressed, which led to uniformized interior stress and effectively inhibited microcracks during cycling. Consequently, HE-NM showed high thermal and structural stability with an initial discharge capacity of 206.35 mAh g–1 at 0.1 C and a retention of 76% after 100 cycles at 1 C, which showed a great advantage over the pristine NM (63%). This work provided a strategy for the stabilization of the NM cathode, which provided insight for the development of high-performance LIBs.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 能源存储
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BRAZILIAN JOURNAL OF CHEMICAL ENGINEERING · 2024 · IF 1.5

Preparation of layered high nickel cobalt-free LiNi0.8Mn0.17Fe0.03O2 cathode material for lithium-ion batteries

Su Yongyou,Zhu Bowen,Zhang Yingjie,Meng Qi,Dong Peng

With the rapid development of the global economy, energy crisis and environmental protection problems are in urgent need of solution. And the development of energy-saving and new energy vehicles is an inevitable trend to improve the energy structure, alleviate the conflict between oil supply and demand, and improve the living environment of human beings. Layered high nickel material is considered as one of the most promising cathode materials for power batteries because of its high energy density, high platform potential and good rate capability. However, it has problems such as high dependence on cobalt resources and poor cycling stability. In this paper, the preparation of layered high nickel cobalt-free cathode materials is investigated. Because Fe element has the advantages of large reserves and low price. At the same time, Fe makes the layered structure of the positive electrode more stable. In this paper, LiNi 0.8 Mn 0.17 Fe 0.03 O 2 (Li/TM = 1.01, 1.03, 1.05) materials with different Li/TM ratios were prepared by solid-phase method to investigate the effects of different Li/TM ratios on the structural and electrochemical properties of LiNi 0.8 Mn 0.17 Fe 0.03 O 2 materials. The results show that the materials synthesized with different Li/TM ratios have a layered structure. When the Li/TM ratio is 1.03, the crystal structure is the best and the degree of Li/Ni mixing is the least. The electrochemical performance study shows that the synthesized materials have the optimal electrochemical performance at the Li/TM ratio of 1.03. The electrochemical behavior during lithium embedding/delithiation was also investigated by quasi-in situ XRD, dQ/dV and CV tests. This study will provide some reference and guidance for the development and application of next-generation low-cost cobalt-free lithium-ion batteries.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 能源科学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-12 · IF 15.7

Electronic structure formed by Y2O3-doping in lithium position assists improvement of charging-voltage for high-nickel cathodes

Wang Shijie,Liang Kang,Zhao Hongshun,Wu Min,He Junfeng,Wei Peng,Ding Zhengping,Li Jianbin,Huang Xiaobing,Ren Yurong

High-capacity power battery can be attained through the elevation of the cut-off voltage for LiNi 0.83 Co 0.12 Mn 0.05 O 2 high-nickel material. Nevertheless, unstable lattice oxygen would be released during the lithium deep extraction. To solve the above issues, the electronic structure is reconstructed by substituting Li + ions with Y 3+ ions. The dopant within the Li layer could transfer electrons to the adjacent lattice oxygen. Subsequently, the accumulated electrons in the oxygen site are transferred to nickel of highly valence state under the action of the reduction coupling mechanism. The modified strategy suppresses the generation of oxygen defects by regulating the local electronic structure, but more importantly, it reduces the concentration of highly reactive Ni 4+ species during the charging state, thus avoiding the evolution of an unexpected phase transition. Strengthening the coupling strength between the lithium layers and transition metal layers finally realizes the fast-charging performance improvement and the cycling stability enhancement under high voltage.

CAS / MDL: 1310-65-2
研究领域: 材料科学 · 电化学
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Energy Storage Materials · 2021 · IF 17.789

In-built ultraconformal interphases enable high-safety practical lithium batteries

Yu Wu,Xuning Feng,Xiang Liu,Xuefeng Wang,Dongsheng Ren,Li Wang,Min Yang,Yongling Wang,Weifeng Zhang,Yalun Li,Yuejiu Zheng,Languang Lu,Xuebing Han,Gui-Liang Xu,Yang Ren,Zonghai Chen,Jitao Chen,Xiangming He,Khalil Amine,Minggao Ouyang

There is an urgent need for high-safety and high-energy lithium-ion batteries to satisfy the rapidly increasing need for energy storage. Nickel-rich layered cathodes have been at the forefront of the revolution for batteries due to their relatively high capacity and low cost. However, with the increase of nickel content, the batteries suffer from severe safety concerns, which caused by thermal runaway. Here we show that the ultraconformal cathode-electrolyte interphase (CEI) protective skin with high inorganic content dramatically enhances the safety of high-energy practical Li-ion pouch cells. We find that the robust CEI skin significantly improves the intrinsic thermal stability, mitigates the evolution of oxygen resulting from phase transition, and effectively suppresses the associated parasitic reactions between the delithiated cathodes and electrolyte. The in-situ CEI engineering strategy is simple and suitable for practical industrial manufacture, and it provides design ideas for aggressive nickel-rich cathodes towards safe and high-energy batteries.

研究领域: 材料科学 · 能源存储
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CANADIAN METALLURGICAL QUARTERLY · 2024 · IF 1.3

Recovery of nickel and iron from ferronickel powder and high nickel matte via the atmospheric leaching-hematite precipitation process

Xiaohua Peng,Xin Jin,Yong Zhen,Bo Yang,Chang Wei,Xingbin Li,Zhigan Deng,Minting Li

This study introduces a novel synergistic leaching process for ferronickel powder and high nickel matte, enabling the atmospheric leaching and the hematite precipitation process to mitigate carbon emissions associated with the treatment of Ni laterite. The results indicated that following seven cycles of synergistic leaching, the Ni2+ concentration in the solution exceeded 80 g/L, compared with the 15 cycles required for non-synergistic leaching. Optimal leaching conditions included a temperature range of 80°C−95°C, a stirring speed of 300 rpm, an initial H2SO4 concentration of 100 g/L, and a reaction time of 8 h, maintaining a final pH of 3.5−4.5, and an excess of ferronickel powder. Leaching successfully extracted Ni and Fe from ferronickel powder, with Cu2+ in the solution being reduced and enriched in the leaching residue. For the hematite precipitation process, optimal conditions involved a temperature of 200°C, a stirring speed of 500 rpm, a reaction time of 3 h, and an addition of 20 g/L of high Ni matte. The Fe removal efficiency exceeded 86%, resulting in hematite products that contained 61.15% Fe, 0.60% Ni and 1.48% S. These products can be commercially utilised, either sold to cement plants or utilized as raw materials for ironmaking.

CAS / MDL: 12054-48-7
研究领域: 冶金工程 · 环境科学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

High voltage electrochemical performance of ultrahigh-Ni cathode via in situ constructed nano-LiF and CNT composite cathode electrolyte interphase layer

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.

CAS / MDL: 308068-56-6 616-38-6
研究领域: 材料科学 · 电化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 167 ·期 16 ·160557 · IF 4.316

Gradient-Regeneration of Li(Ni0.9Co0.05Mn0.05)O2 from Spent LiCoO2 lithium-Ion Battery

Guange Wang,Tong Wu,Borui Liu,Shanshan Gong,Qing Huang,Yuefeng Su,Feng Wu,Ryan M. Kelly

Considering that lithium-ion battery (LIB) is still an indispensable and important component of energy storage materials, the sustainable post-processing of spent LIBs in labs or enterprises becomes a tricky problem. Herein, a novel scheme is proposed to dissert the recycling of the spent LIBs. The LIB is recycled into Li(Ni0.9Co0.05Mn0.05)O2 (NCM90) cathode material with high specific capacity by introducing an innovative hydrometallurgy-coprecipitation treatment method. The spent LiCoO2 (LCO) cathode material is firstly leached by sulfuric acid, and the leachate is gradient used as the raw materials to resynthesize high-nickel NCM material by adjusting the leachate dosage to about 50%. Interestingly, when the dosage exceeds 50%, the crystal structure aggravates, and Li+/Ni2+ mixing improves. The specific capacity of regenerated battery is 181.4 mAh g−1 at 0.5 C (1 C = 200 mAh g−1) and the capacity retention achieves 93.2% after 100 cycles. The reasons can be attributed to the cation mixing and crystal strucure and the small amount of Al doping. In conclusion, this combined method recycling of LIBs has huge potential value for environment protection and production.

研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Lanthanum doping and surface Li3BO3 passivating layer enabling 4.8 V nickel-rich layered oxide cathodes toward high energy lithium-ion batteries

Min Xu,Junjie Lu,Zhefei Sun,Ming Yang,Bifu Sheng,Minfeng Chen,Jizhang Chen,Qiaobao Zhang,Xiang Han

Single crystalline Ni-rich layered oxide cathodes show high energy density and low cost, have been regarded as one of the most promising candidates for next generation lithium-ion batteries (LIBs). Extending the cycling voltage window will significantly improve the energy density, however, suffers from bulk structural and interfacial chemistry degradation, leading to rapidly cycle performance deterioration. Here, we propose a dual-modification strategy to synthesize La doping and Li 3 BO 3 (LBO) coating layers modified LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) by a facile one-step heating treatment processing. In-situ EIS and XRD, ex-situ XPS techniques are applied to demonstrate that the La diffused amorphous domains and Li 3 BO 3 passivating layers dampen the lattice distortion, enhance the interfacial chemistry behavior as well as lithium ion transportation kinetics. Specifically, surface La doping amorphous domains successfully suppress the intense lattice stress and volume changes induced by the phase transitions during lithiation/delithiation, thus avoiding the intergranular crack and enhancing the mechanical stability of the material. Moreover, the LBO layer formed by the consumption of residual lithium prevents successive parasitic reactions at the interface as well as provides rapid Li-ion diffusion channels. Furthermore, the coating layer also diminishes the residual lithium compounds, increasing the atmosphere stability and safety of LIBs. Consequently, the La doping and LBO coating NCM811 exhibits an exceptional initial specific capacity (230.6 mAh/g) at 0.5C under a high cutoff voltage of 4.8 V, and a 73.8 % capacity retention following 100 cycles. In addition, a superior specific capacity of 133.8 mAh/g is provided even at a high current density (4C). Our work paves a promising road to tackle the integral structure deterioration and interfacial instability of Ni-rich cathodes.

研究领域: 材料科学 · 电化学
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2021 ·Vol. 37 ·期 2 ·280-285 · IF 1.307

Synthesis and Electrochemical Investigation of O3-Type High-nickel NCM Cathodes for Sodium-ion Batteries

Chen Yawei,Wang Shiyang,Jie Yulin,Lei Zhanwu,Cao Ruiguo,Jiao Shuhong

Sodium ion batteries(SIBs) are promising energy storage devices for smart grid applications due to their low cost and the high abundance of sodium, but few cathode materials of SIBs with high energy density are available for practical applications. Herein, a series of NaNCM ternary materials(NCM=nickel-cobalt-manganese) is obtained by solid- phase reaction with well-regulated temperature and other reaction conditions. XRD results show that impure NiO phase is more likely to occur under high nickel content. The cross-section SEM indicates that the primary particles in the electrode materials are radially distributed along the radial direction, and the internal porous structure is conducive to the infiltration of electrolyte. The initial specific capacities of Na[Ni 0.68 Co 0.10 Mn 0.22 ]O 2 (NaNCM712), Na[Ni 0.6 Co 0.2 Mn 0.2 ]O 2 (NaNCM622) and Na[Ni 0.4 Co 0.3 Mn 0.3 ]O 2 (NaNCM433) at 0.2 C are 165.5, 153.1 and 146.8 mA·h/g, and the corresponding capacity retention rates are 63.2%, 78.5% and 71.7% after 100 cycles. NaNCM712 possesses the highest initial specific capacity, and NaNCM433 delivers the best rate capability. The rate capabilities of high-nickel and low-cobalt NaNCM cathodes need to be further improved. Moreover, ex-situ XRD pattern reveals the structure evolution (from O3 type to P2 type) during a long cycling charge and discharge process.

研究领域: 材料科学 · 电化学
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2025 ·Vol. 41 ·期 2 ·333-342 · IF 3

Enhancing Structural Stability and Electrochemical Performance of Ultra-high Ni-rich Co-free Cathode via MgHPO4 Dual-functional Modification

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.

CAS / MDL: 7782-75-4
研究领域: 材料科学 · 电化学
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Materials Today Communications · 2025 · IF 4.5

Synergistic effect of Na and B co-doping on the electrochemical properties of LiNi0.865Co0.095Al0.04O2 cathode materials for Li-ion batteries

Wujie Ge,Yuanxiang Fu,Chaonan Wang,Lirong Yan,Qi Feng,Bing Yan,Xiang Li

The high-nickel cathode material LiNi 0.865 Co 0.095 Al 0.04 O 2 (NCA) has garnered significant attention due to its high energy density and cost-effectiveness in production. However, this material is also prone to rapid capacity degradation, primarily due to phase transitions occurring during the redox process. In this paper, the co-modification with Na and B cations is employed to stabilize the lattice structure and enhance the electrochemical performance of the NCA material. It can be found that the incorporation of Na and B cations in the lattice can reduce cation mixing, expand the Li-layer spacing and improve crystal stability, thereby increasing the specific capacity and cyclic stability of the NCA material. Specifically, the co-doped NCA-2 sample exhibits a specific capacity of 202.1 mAh/g at 0.1 C and maintains a capacity retention of 78.75 % at 1 C after 300 cycles, representing a substantial improvement over the pristine material (187.2 mAh/g and 61.68 % capacity retention). Moreover, at a current density of 10 C, the co-doped NCA-2 sample demonstrates a high specific capacity of 133.9 mAh/g, compared to 110.1 mAh/g for the pristine material. The Na/B co-doping strategy presented in this study offers a straightforward method to improve the cyclability and rate behavior of cathode materials, highlighting its potential for commercial applications.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Preparation of LiNi0.8Co0.1Mn0.1O2 electrodes by 3D printing

Lijie Zhai,Mengting Lv,Mengmeng Cong,Tao Lin,Nan Meng,Fang Lian,Huiping Shao

The LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) electrodes are successfully prepared by 3D gel printing (3DGP) technique in this study. The results show that when the slurry with 45 % solid content was squeezed out of the needle, the viscosity of the printing slurry was 1.54 Pa s at the shear rate of 660 s −1 , which shows that the printing slurries are suitable for 3DGP. At the same time, when the inner diameter of the printing needle is 0.25 mm, the air pressure is 0.40 MPa and the printing speed is 4.60 mm s −1 , the structure of printing electrode is complete. The electrochemical measurement results show the printed NCM electrode with 231 μm printing line spacing has a higher capacity of 169.80 mAh g −1  at 4C, a specific capacity of 103.9 mAh g −1  at 1C after 500 cycles and an energy density of 232 Wh kg −1 , which shows that the high specific capacity and good cycling stability exhibited by NCM electrodes fabricated by 3DGP.

研究领域: 材料科学 · 电化学 · 能源存储 · 增材制造
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