ELECTROCHIMICA ACTA
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2019
·
IF 5.383
Aijia Wei,Wen Li,Qian Chang,Xue Bai,Rui He,Lihui Zhang,Zhenfa Liu,Yanji Wang
Mg 2+ /F − co-doped LiNi 0.5 Mn 1.5 O 4 cathode material was synthesized by a facile one-step solid-state process. The effect of Mg 2+ /F − co-doping on grain morphology, phase structure, and electrochemical properties was studied by a series of characterizations. Scanning-electron-microscopy images show that Mg 2+ /F − co-doped LiNi 0.5 Mn 1.5 O 4 (denoted LNMO-MF) particles grow larger than pure LiNi 0.5 Mn 1.5 O 4 particles. X-ray diffraction, Raman spectra , Fourier transformation infrared spectroscopy , X-ray photoelectron spectroscopy, and cyclic-voltammetry tests indicate that all samples mainly display a Fd -3m space group and more Mn 3+ ions in the LNMO-MF sample after Mg 2+ /F − co-doping, which is conducive to increasing the cationic disorder degree and enhancing the electronic conductivity of electrode material. Results show that the LNMO-MF cathode material delivers an excellent rate performance with discharge capacities of 142, 144, 140 136, 132, 124, 115, and 100 mAh g −1 at 0.2, 0.5, 1, 2, 3, 5, 7, and 10C (1C = 140 mAh g −1 ), respectively. Remarkably, LNMO-MF also shows cycling stability with a capacity retention of 86.2% at 5C after 400 cycles, which is much higher than that of pure LiNi 0.5 Mn 1.5 O 4 (67.7%). The improvement of LNMO-MF's electrochemical properties could be ascribed to the Mg 2+ /F − co-doping, delivering a more stable structure, better crystallinity , the highest Li + diffusion coefficient , and the lowest charge-transfer resistance.
研究领域:
材料科学
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电化学
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无机非金属材料
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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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功能材料
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Youguo Huang,Yan Li,Chunlei Tan,Zhikang Huang,Qichang Pan,Youqi Chu,Fenghua Zheng,Hongqiang Wang,Qingyu Li
LiNi0.5Mn1.5O4 (LNMO) is considered one of the most promising cathode materials for high-energy-density lithium-ion batteries (LIBs). However, the practical application of the LNMO cathode is seriously limited by the poor cycling performance. Hence, methyl phenyl sulfone (MPS) is investigated as an electrolyte additive to modify the cathode–electrolyte interphase and furthermore enhance the electrochemical performance of the LNMO cathode at a high voltage (5 V class). Results evidenced that the cycling performance of LNMO/Li cells was improved remarkably and with a high capacity retention of 89.8% after 400 cycles at 1 C in the 0.1 wt % MPS-containing electrolyte. Subsequently, the rate capability is also significantly improved with a high capacity of 110.2 mAh g–1 even at 5 C. Furthermore, the reason for the much-improved electrochemical performance of the LNMO/Li cell is further investigated in detail. Our investigation reveals that MPS additive can alleviate the decomposition of LiPF6 and is oxidized to form a protective layer, which inhibits the decomposition of electrolyte and dissolution of transition metals and then stabilizes the structure of the LNMO cathode during the cycling process. As a result, such a functional additive provides a cost-efficient choice to achieve the high performance of the LNMO cathode in high-voltage LIBs.
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JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Jingjun Liu,Mingliang Yuan,Huiyang Liu,Zhen Li,Lianghua Wang,Junqing Yan,Jing Peng,Shengwen Ou,Jingyue Xu
By employing a modification strategy that involves Mg 2+ doping and Cu coating on the LiNi 0.5 Mn 1.5 O 4 (LNMO) cathode material , along with a composite of zeolite and graphene as an additive in conductive carbon black, we successfully develop multifunctional cathode materials with internal oxygen self-absorption capabilities. We conduct various tests, including morphology and structure analysis, oxygen release and absorption evaluation, weight loss examination, and electrochemical performance assessment, on the prepared samples. Results reveal that Mg 2+ doping restrains the release of lattice oxygen from LNMO materials, thereby enhancing their structural stability. Cu coating and additives play a crucial role in absorbing released oxygen, preventing combustion, and inhibiting side reactions. The micropores of zeolite in the additive adsorb and immobilize gas molecules, reducing the release and diffusion of pyrolysis products, which exhibit flame retardancy properties . Additionally, the presence of graphene, as a highly conductive material , further improves the electrochemical performance of the cathode material. Remarkably, even after 500 cycles at a 1C rate, the modified cathode material with additives maintains a capacity of 115.03mAh⋅g −1 (93.29 % capacity retention). Overall, the demonstrated spinel-type cathode materials exhibit exceptional structural stability, thermal stability, and electrochemical performance, making them promising candidates for advanced lithium-ion batteries.
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高影响因子
ACS Applied Materials & Interfaces
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2019
·
IF 8.456
Tao Huang,Xiangzhen Zheng,Ying Pan,Qiaohong Li,Maoxiang Wu
Tributyl borate (TBB) is studied as a protective additive that enhances the interfacial stability of a LiNi0.5Mn1.5O4 cathode/electrolyte at 5 V and 55 °C. Upon addition of 0.5 vol % TBB to the electrolyte (1.0 M LiPF6/EC:EMC:DMC, 1:1:1 wt %), the LiNi0.5Mn1.5O4/Li cell maintains a discharge capacity of 99.4 mAh g–1 at the 50th cycle at 55 °C, compared to that of the electrolyte without an additive, i.e., 36.6 mAh g–1. Furthermore, the TBB-enhanced Li/LiNi0.5Mn1.5O4 cell exhibits a higher discharge capacity of 96 mAh g–1 at 3C, whereas the cell without TBB delivers only 84 mAh g–1. Theoretical calculations and differential capacity (dQ/dV) versus voltage (V) analysis show that TBB improves the electrochemical performance at 5 V and 55 °C by preferentially oxidizing on the LiNi0.5Mn1.5O4 surface. The results obtained from electrochemical impedance spectroscopy, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, and inductively coupled plasma-mass spectroscopy measurements reveal that TBB generates a thin, less resistive film on the surface of LiNi0.5Mn1.5O4. This TBB-derived film inhibits the decomposition of the carbonate solvent, while suppressing the dissolution of Ni and Mn ions from LiNi0.5Mn1.5O4.
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DOI
PubMed
高影响因子
Scientific Reports
·
2025
·Vol. 15
·期 1
·1-14
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IF 3.9
Wei Aijia,Yang Yuqi,Mu Jinping,He Rui,Li Xiaohui,Zhang Haipeng,Liu Zhenfa,Wang Shasha,Zheng Yong,Mei Shuxing
The instability of the electrode/electrolyte interface and the metal-ions dissolution of high-voltage LiNi 0.5 Mn 1.5 O 4 (LNMO) material lead to significant degradation of cycling performance, thereby limiting the large-scale application of LNMO-based batteries. Here, inorganic Mg/Ca/Sr-contained phosphates (MgHPO 4 , CaHPO 4 , and SrHPO 4 ) are used individually as functional additives of standard electrolytes to enhance the cycling performance of LNMO. Combined with theoretical calculations, a series of electrochemical measurements and characteristics corroborate that the MgHPO 4 is the optimal additive and can preferentially undergo oxidation and reduction decomposition over carbonate solvents. Electrochemical results reveal that the LNMO/Li half-cell containing the MgHPO 4 additive shows a capacity retention of 91.9% after 500 cycles at 5 C, higher than that obtained with STD (76.5%). In addition, the LNMO/graphite (Gr) full-cell with MgHPO 4 additive increases the capacity retention from 70.8 to 78.0% after 100 cycles at 0.5 C. The addition of MgHPO 4 allows a thin, uniform, and conductive cathode-electrolyte interphase (CEI) and solid-electrolyte interphase (SEI) film to be formed on the LNMO cathode and graphite anodes. Furthermore, the preferential reduction of MgHPO 4 inhibits the lithium dendritic growth and enables the formation of a more stable SEI on the Li anode. Besides, the MgHPO 4 additive serves as a scavenger of detrimental HF, thus suppressing the Ni/Mn ions dissolution and improving the structural stability of LNMO. This study provides a cost-effective strategy involving the use of an inorganic additive for improving the electrochemical performance of high-voltage lithium-ion batteries.
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高影响因子
Crystals
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2017
·Vol. 7
·期 9
·275
·
IF 1.566
Yang Shu,Wenchao Yan,Haisong Wang,Jicheng Jiang,Deye Sun,Xiaodi Ma,Yongcheng Jin
A series of LiNi0.5Mn1.5O4(LNMO) samples were synthesized by adjusting the molar ratio of (NH4)2CO3to Na2CO3in a mixed precipitant for evaluating the effects of ammonia from (NH4)2CO3as a complexing agent and Na2CO3as a precipitant on the morphology and electrochemical performances of LNMO. In this research, a rapid precipitation method followed by hydrothermal treatment was used to prepare the precursors of LNMO, and different molar ratios (0:1, 1:2, 1:1, 2:1, 1:0) of (NH4)2CO3to Na2CO3were used for mixed precipitants. The test results revealed that the cathode material exhibits the best electrochemical performance when the molar ratio of (NH4)2CO3to Na2CO3is set at 1:2, displaying a specific discharge capacity of 129.4 mA h g−1at 0.5 C and a capacity retention of 82.3% after 200 charge–discharge cycles. In addition, it still shows a high rate performance with a discharge capacity of 112.7 mA h g−1at 10 C and 98.8 mA h g−1at 20 C, which is attributed to an accurate Ni/Mn ratio, smaller primary particle sizes and a porous spherical morphology.Keywords:rapid precipitation;hydrothermal treatment;mixed precipitants;spherical morphology
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Materials Today
·
2025
·
IF 22
Liang Li,Tao Yang,Kaixiang Ren,Xinchun Song,Shilin Wu,Hai-Wen Li,Zhipeng Jiang,Mengjun Sun,Yongtao Li
Lithium-LiNi 0.5 Mn 1.5 O 4 (LNMO) batteries are considered promising candidates for high-energy–density storage due to their high operational voltage and low cost. However, existing electrolytes typically fail to balance high-voltage stability with electrode compatibility, thereby limiting their performance under practical conditions. In this study, we present a synergistic inhibition engineering in which silyl additives—triethylsilyl trifluoromethanesulfonate (TESOTf) and tris(trimethylsiloxy)boron (TMSB)—are incorporated into a conventional carbonate electrolyte, leading to stable cycling of Li-LNMO batteries at voltages as high as 4.9 V. Through in situ techniques and theoretical simulations, we demonstrate that TMSB immobilizes free PF 6 − ions in the electrolyte, while TESOTf preferentially consumes trace amounts of water, thereby shifting the hydrolysis reaction pathway of PF 6 − and reducing side reactions at the cathode. Electrochemical tests show that the addition of small quantities of TESOTf and TMSB significantly enhances the rate capability (10C for 85.2 mAh g −1 ), cycling stability (5C for 500 cycles), and high-temperature performance (60 °C, 5C for 300 cycles) of Li-LNMO cells. More importantly, a practical 3 Ah Li-LNMO pouch cell containing these additives demonstrated stable cycling under practical conditions (20 mg cm −2 , 20 μm Li, 2 g Ah −1 ), achieving an energy density exceeding 300 Wh kg −1 .
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2026
·
IF 3.6
Pengcheng Chai,Qian Zhang,Shengli Chen,Jiangfeng Qian
Lithium nickel manganese oxide (LiNi 0.5 Mn 1.5 O 4 , LNMO) is a promising cobalt-free cathode operating at ∼4.7 V primarily through the Ni 4+ /Ni 2+ redox couple. Deep discharging to 2.30 V can activate the electrochemically inert Mn, which contributes additional capacity and improves energy density. However, repeated cycling over such a wide-voltage window (2.30–4.95 V) imposes severe mechanical stress and dynamic interphase degradation. Here, we demonstrate that these challenges are effectively mitigated by employing λ -carrageenan (CGN) as a multifunctional binder that maintains the electrode integrity and regulates cathode–electrolyte interphase (CEI) evolution. The resulting LNMO cathode achieves a high specific capacity of 186 mAh g −1 and an energy density of 755 Wh kg −1 within 2.30–4.95 V through simultaneous activation of Ni and Mn redox. Notably, the CGN/LNMO electrode retains 87.7% of its capacity after 200 cycles at 0.5C, compared to only 29.6% for a conventional PVDF/LNMO electrode. This binder-enabled interfacial regulation strategy establishes an effective pathway toward stable wide-voltage operation of high-energy-density cathode materials. Graphical The use of λ -carrageenan (CGN) as a binder with robust hydrogen-bonding interactions for LiNi 0.5 Mn 1.5 O 4 (LNMO) during wide-voltage cycling leads to a homogeneous coating that prevents rock-salt phase formation and develops into a stable CEI, enabling stable cycling within 2.30–4.95 V.
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Chunlei Tan,Zhikang Huang,Yu Li,You Li,Yujie Zou,Xiaohui Zhang,Lisan Cui,Feiyan Lai,Guanhua Yang,Chenggui Jing,Hongqiang Wang,Qingyu Li
The poor cyclic stability is the key point to restricting the commercial application of LNi 0.5 Mn 1.5 O 4 -based lithium-ion batteries (LNMO-based LIBs) on high voltage (5 V-class). Once the working voltage is over 4.3 V, the parasitic reactions on the LNMO interphase will be the trigger for a series of problems such as the continuous decomposition of electrolytes and dissolution of transition metal ions. The glyceryl triacetate (GT) has been used as a functional additive to reconstruct a cathode electrolyte interphase (CEI) film to suppress the parasitic reactions and safeguard the LNMO structure. Compared to the influence of GT and propionic anhydride (PA) on the electrochemical performance of LNMO on high voltage, the LNMO/Li cell with GT exhibits exciting discharge capacity retention of 84.9 % compared with PA (17.6 %) and base electrolyte (BE, 8.6 %) after 500 cycles at 1C. The LNMO/Li cell with GT also has a remarkable rate performance in which capacity retention of 5C/2C is 85.7%, higher than 0.5 wt% PA (75.5%) and BE (62.1%). By characterizations, it is reasoningly demonstrated that the GT not only can be preferentially oxidized to form a robust CEI film on the LNMO surface to prevent the parasitic reaction but also rapidly capture the free transition metal ions and bind trace H 2 O in the electrolyte to improve the stability of LIBs. Simultaneously, the electrons from the carboxyl group of GT occupy the d-orbital of transition metal from LNMO, further effectively reducing the activity of LNMO. Particularly, the glycerol generated by the reaction of GT with H 2 O can effectively capture HF, H 2 O, and other small molecules under hydrogen-bond interaction, thereby improving the stability of LNMO LIBs.
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高影响因子
Energy Technology
·
2020
·Vol. 8
·期 10
·2000671
·
IF 3.404
Huimin Shang,Gongchang Peng,Wenjing Liu,Huan Zhang,Wenchao Niu,Yingling Liao,Meizhen Qu,Zhengwei Xie
Pyrene (PY) is first used as an additive to improve the cyclic stability of LiNi 0.5 Mn 1.5 O 4 at high cutoff voltage. After 300 cycles at room temperature (≈25 °C) and 100 cycles at elevated temperature (≈55 °C), the capacity retention of Li/LiNi 0.5 Mn 1.5 O 4 cells is 93.1% and 92.68% in the electrolyte containing 0.0025 wt% PY. However, in the base electrolyte, the capacity retention of the cells is 84.7% and 88.12%. The improved capacity retention is due to a thin and even cathode electrolyte interphase (CEI) film containing the poly-PY on surface of LiNi 0.5 Mn 1.5 O 4 , which reduces the oxidation reaction of electrolyte, the dissolution of transition metal, and the interface impedance in subsequent cycles. In addition, the cross-talk effect between the positive and negative electrodes is effectively avoided. The film derived from PY also improves the rate performance of cell at room temperature.
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DOI
高影响因子
AIP Advances
·
2019
·Vol. 9
·期 2
·
IF 1.579
Li Sheng,Lan Lifang,Lu Lu,Lu Yan,Li Shaofang,Li Jun,Pan Chunyang,Zhao Fenghua
To investigate the effect of Ce doping on structure and the electrochemical properties of spinel LiNi 0.5 Mn 1.5 O 4 , especially the cycling performance at high temperature, spinel cathode materials LiNi 0.5-0.5x Mn 1.5-0.5x Ce x O 4 (x = 0, 0.01, 0.02, 0.03) were prepared by the sol-gel method for use in lithium ion batteries. For this purpose a half-cell was assembled with a lithium metal anode and a full-cell was paired with graphite. The characterization and analysis of the prepared LiNi 0.5-0.5x Mn 1.5-0.5x Ce x O 4 (x = 0, 0.01, 0.02, 0.03) composites revealed that all of the samples had a disordered spinel octahedron structure, and that the purity of the phase increased after appropriate Ce doping. Compared to the pristine sample, the prepared LiNi 0.495 Mn 1.495 Ce 0.02 O 4 , (x = 0.02) had outstanding electrochemical performance with an initial capacity of 133.8 mAh/g, and 131.9 mAh/g at 1 C and 55 °C after 50 cycles, and maintained a capacity retention value of 98.6% at 1 C and 25 °C at the 100th cycle. The introduction of Ce as dopant improved the electrochemical performance of LiNi 0.5 Mn 1.5 O 4 as a result of the synergistic effects of stronger structural stability, higher lithium ion diffusion coefficient, and lower electrochemical polarization.
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高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Weikang Mei,Guobao Xu,Hongyu Wang
Li4Ti5O12 (LTO)/LiNi0.5Mn1.5O4 (LNMO) batteries have appealing features, such as suitable energy density and high safety. A proper binder of the LNMO cathode and electrolyte can improve the performance of batteries. Herein, we first combined the polyacrylic acid (PAA) binder with an ester-based electrolyte due to their homologous structure. This system has better performance than other binders of LNMO cathode, like poly(vinylidene fluoride) (PVDF), styrene–butadiene rubber (SBR), and polytetrafluoroethylene (PTFE). In the methyl acetate (MA) electrolyte, the LTO/LNMO battery with the PAA binder exhibited the highest discharge capacity (137 mAh g–1 at 0.5 C) and the best rate performance (112 mAh g–1 at 5 C). In addition, MA boosted the low-temperature performance of this battery, which can work at −40 °C with a remarkable reversible capacity of 90 mAh g–1 and a discharge capacity of 140 mAh g–1.
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