Energy Storage Materials
·
2025
·
IF 20.2
Ridong Hu,Chong Mao,Hao Zhuo,Xiaobing Dai,Lewen Yang,Xugang Shu,Yang Li,Zhanqiang Li,Wenhong Ruan,Fujie Yang,Xudong Chen
The precarious interfacial chemistry between the electrode and electrolyte is the determining step that restricts the long cycle life of Ni-rich-based Li-metal batteries. Here we show that the robust cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers can be engineered by tuning the spatial linking structure of dipentacyclic anhydride (DPA) additives. Specifically, an inorganic-rich CEI/SEI layer induced by CBDA (a DPA featuring a quaternary ring spatial linking structure) exhibits superior Li + interfacial kinetics and an ultra-stable cycle performance, outperforming the other systems. As a result, the NCM811ǁLi cells containing CBDA show excellent long-term performances, even under high voltage, high load, and high charge-discharge current density, respectively. The coin-cell using a low-loading cathode exhibits 129 mAh g- 1 discharged capacity for over 200 cycles at a 6 C rate. Moreover, The high-loading cathode retains 80 % capacity after 312 cycles at 1.0 C. Furthermore, the NCM811ǁLi pouch cell demonstrated a capacity retention rate of 99.8 % after 50 cycles. Prolonged stable cycling for 900 cycles (93 % capacity retention) in an NCM811ǁGraphite pouch cell is enabled by CBDA. The DPA-based additives in this work offer a highly promising and feasible route to achieving a long-term and high-capacity lithium battery featuring a Ni-rich cathode.
研究领域:
电化学储能
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Zeng,Sheng-Qi Su,Ying-Min Qin,Jing-Zhe Wu,Jiang-Nan Ke,Yong-Gang Sun,Xi-Jie Lin
Ni-rich layered oxides offer numerous advantages such as high discharge capacity, cost-effectiveness, and environmental friendliness, making them the mainstream cathodes for high-energy density lithium-ion batteries. However, their widespread commercialization is hindered by critical challenges in cycling performance, stemming from unstable interface and structure, particularly at elevated charge cut-off voltages. Herein, a dual-modification strategy combining La doping and La 4 NiLiO 8 coating was proposed to synergistically enhance the surface/interface and structure stability of the LiNi 0.83 Co 0.11 Mn 0.06 O 2 (referred to as NCM83) cathode. Unlike conventional methods, a well-designed La(OH) 3 coating pretreatment was employed on the Ni 0.83 Co 0.11 Mn 0.06 (OH) 2 precursor. This pretreatment aimed to facilitate the in-situ formation of La doping and La 4 NiLiO 8 during the lithiation of the coated precursor, while ensuring desired uniformity of the La 4 NiLiO 8 coating and La doping. This dual-modification strategy integrated the advantages of both La doping and La 4 NiLiO 8 coating, demonstrating excellent capability to improve the overall performance of NCM83. The La doping, acting as a pillar, not only strengthened the layered structure of the cathode to mitigate volume changes, but also enhanced Li + diffusion by broadening the c axis spacing. The La 4 NiLiO 8 coating efficiently protected the cathode from H 2 O/CO 2 attack and electrolyte erosion, while also facilitating Li + transport owing to its favorable Li-conductive properties. Such a dual-modification strategy significantly enhanced the electrochemical performance of NCM83, as demonstrated by the excellent long-term cyclic stability, rate capability, and thermal stability at a high charge cut-off voltage of 4.5 V. This work highlighted the benefits of integrating elemental doping and surface coating, while offering a promising synthetic protocol for straightforward and effective dual-modification of various 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
ACS Nano
·
2024
·
IF 15.8
Shiming Chen,Guorui Zheng,Xiangming Yao,Jinlin Xiao,Wenguang Zhao,Ke Li,Jianjun Fang,Zhuonan Jiang,Yuxiang Huang,Yuchen Ji,Kai Yang,Zu-Wei Yin,Meng Zhang,Feng Pan,Luyi Yang
Coupling Ni-rich layered oxide cathodes with Si-based anodes is one of the most promising strategies to realize high-energy-density Li-ion batteries. However, unstable interfaces on both cathode and anode sides cause continuous parasitic reactions, resulting in structural degradation and capacity fading of full cells. Herein, lithium tetrafluoro(oxalato) phosphate is synthesized and applied as a multifunctional electrolyte additive to mitigate irreversible volume swing of the SiOx anode and suppress undesirable interfacial evolution of the LiNi0.83Co0.12Mn0.05O2 (NCM) cathode simultaneously, resulting in improved cycle life. Benefiting from its desirable redox thermodynamics and kinetics, the molecularly tailored additive facilitates matching interphases consisting of LiF, Li3PO4, and P-containing macromolecular polymer on both the NCM cathode and SiOx anode, respectively, modulating interfacial chemo-mechanical stability as well as charge transfer kinetics. More encouragingly, the proposed strategy enables 4.4 V 21700 cylindrical batteries (5 Ah) with excellent cycling stability (92.9% capacity retention after 300 cycles) under practical conditions. The key finding points out a fresh perspective on interfacial optimization for high-energy-density battery systems.
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
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Zhikun Zhao,Ziyue Wen,Chunli Li,Yin Ding,Ying Jiang,Feng Wu,Borong Wu,Shi Chen,Daobin Mu
Herein we combine X-ray photoelectron spectroscopy, AC impedance experiments and high resolution transmission electron microscopy to provide new insight into the degradation mechanism of a nickel-rich cathode material under different charge voltages. The degradation is closely related to the charge/discharge cut-off voltage. We use a simple in-situ method to generate a stable Li 2 WO 4 layer with a thickness of ∼10 nm on the LiNi 0.6 Co 0.2 Mn 0.2 O 2 surface during the calcination process using (NH 4 ) 2 WO 4 . This decorated layer prevents side reactions and reduces formation of the insulators LiF and Li 2 CO 3 on the surface of the particles. Electrochemical impedance spectroscopy shows that the Li 2 WO 4 layer has no effect on the interphase film resistance of the cathode/electrolyte, which remains stable during the cycling process. The charge transfer of LiNi 0.6 Co 0.2 Mn 0.2 O 2 is improved a lot by the decorated layer. Transmission electron microscopy shows that increasing amounts of a rock-salt phase substance forms with increasing cut-off voltage, while for the Li 2 WO 4 -decorated sample only a small amount of rock-salt forms on the surface of the cathode material. This study illustrates the relationship between changes in the surface structure with different cut-off voltages and the electrochemical performance, and provides an effective approach to improve the cycling performance of nickel-rich cathode materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2019
·
IF 0
Qingyu Dong,Feng Guo,Zhenjie Cheng,Yayun Mao,Rong Huang,Fangsen Li,Houcai Dong,Qingyong Zhang,Wei Li,Hui Chen,Zhaojun Luo,Yanbin Shen,Xiaodong Wu,Liwei Chen
Ni-rich layered oxides (LiNixMnyCozO2, x ≥ 0.6, x + y + z = 1) are promising positive electrode materials for high energy density lithium-ion batteries thanks to their high specific capacity. However, large-scale application of Ni-rich layered oxides is hindered by its poor structural and interfacial stability, especially during cycling at a high cutoff potential (i.e., ≥ 4.3 V, versus Li+/Li). Herein, we demonstrate that lithium difluoro(oxalato)borate (LiDFOB) as a film-forming additive plays a dual role on the electrode|electrolyte interphase formation in a LiNi0.83Mn0.05Co0.12O2||graphite cell, meaning that it can not only be reduced on the graphite negative electrode but also oxidized on the nickel-rich oxide LiNi0.83Mn0.05Co0.12O2 positive electrode cycled at a high cutoff potential (4.4 V, versus Li+/Li) prior to typical carbonate-based electrolyte constituents. As a result, the addition of 1.5 wt % LiDFOB greatly reduces the polarization and improves the cycling stability of the LiNi0.83Mn0.05Co0.12O2||graphite cell, which shows a high discharge capacity of 198 mA h g–1, and more than 83.1% of the initial capacity was retained after 200 cycles at C/3 (the capacity retention obtained at the same cycling condition is only 59.9% for the cell without LiDFOB additive). Furthermore, the employ of LiDFOB additive also significantly suppresses the self-discharge of the LiNi0.83Mn0.05Co0.12O2||Li cell during high-temperature and long-term room-temperature storage at 4.4 V. These electrochemical performance enhancements could be attributed to the participation of LiDFOB in forming a stable and Li+ transfer favorable protective layer that is rich in inorganic boron, fluorine, and carbonate compounds on both the surface of the LiNi0.83Mn0.05Co0.12O2 positive electrode and the graphite negative electrode, thus suppressing the electrolyte decomposition on the positive electrode and negative electrode surfaces and decreasing the dissolution of transition-metal ions from the positive electrode bulk.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Sen Jiang,Xin Xu,Junying Yin,Xuequan Zhu,Lai Wei,Kang Xi,Linghao Zhang,Yuelang Lan,Haihua Wu,Yunfang Gao
Rechargeable lithium metal batteries (LMBs) coupling with Ni-rich cathodes are promising high-energy-density electrochemical energy storage devices. However, the growth of Li dendrites and structural degradation of Ni-rich materials, associated with the erratic electrode-electrolyte interphase (EEI) and corrosion of harmful acidic species from the hydrolysis of LiPF 6 , seriously deteriorate the cycling performance of LMBs with Ni-rich cathodes. Herein, glutaric anhydride (GA) as a multifunctional electrolyte additive is proposed to achieve satisfactory lifespan of LMBs by in situ constructing LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode/Li anode-electrolyte interphases (CEI/AEI), and scavenging corrosive acidic species. The GA-derived CEI/AEI layers are rich in C O species, which can strongly coordinate with the Li anode and delithiated Ni-rich cathode surface . Thus, parasitic reactions of the electrolyte on the aggressive surface of the Ni-rich cathode and Li anode are notably reduced. Furthermore, the problems such as the inner microcrack evolution of NCM811 particles, the growth of Li dendrites and the corrosion of acidic species are well addressed. Consequently, the capacity retention of Li/NCM811 cell is increased from 59.4% to 90.7% after 300 cycles at 1C in the presence of GA, and the Li/Li symmetrical cell with GA exhibits the super-stable cyclic performance of 1400 h at 0.2 mA cm −2 .
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
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sen Jiang,Xin Xu,Junying Yin,Haihua Wu,Xuequan Zhu,Hongtao Guan,Lai Wei,Kang Xi,Yuelang Lan,Linghao Zhang,Yang Qiu,Yunfang Gao
Li metal batteries (LMBs) coupled with Ni-rich materials are promising candidates for next-generation high-energy-density lithium batteries. However, due to the inferior stability of cathode/solid-electrolyte interphases (CEI/SEI) and aggressive chemistry of Ni-rich cathode materials, Li metal anode (LMA) and LiPF 6 -based carbonate electrolytes pose a threat to the achievement of high-energy-density LMBs. Herein, 1-(trimethylsilyloxy)cyclohexene (TMSCH) with functional groups (C=C, Si-O) as a novel multi-functional electrolyte additive is employed to regular the CEI/SEI films on the both Ni-rich cathode materials (LiNi 0.8 Co 0.1 Mn 0.1 O 2 , NCM811) and LMA surface, and scavenge detrimental hydrogen fluoride (HF) to enhance electrochemical performances of the Li/NCM811 batteries. Furthermore, the theoretical calculation, electrochemical measurements and physical characterizations demonstrate the feasibility and effectiveness of the strategy. Specially, the TMSCH-derived SEI film exhibits a hierarchical structure consisting of an organic-rich outer layer and a LiF-rich inner layer. Accordingly, the microcracks generation of NCM811 secondary particles, transition metal ions dissolution, lithium dendrite growth, parasitic reactions and HF generation of electrolyte are effectively addressed. As a result, with existence of the TMSCH additive, the capacity retention of Li/NCM811 batteries at 1C are remarkably enhanced from 68.2% to 84.9% at 30 °C and 64.2% to 85.8% at 45 °C. Furthermore, the Li/Li symmetric cells with TMSCH can stably cycle over 1000 h at 0.2 mA cm −2 and exhibit super-low overpotential of 75 mV at 1 mA cm −2 .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Hanwei Zhang,Xiaoyun Zhang,Tianyi Zeng,Aichun Dou,Panpan Zhang,Mingru Su,Yu Zhou,Yunjian Liu
The application of Ni-rich ternary cathode materials is restricted by the irreversible phase transition and interfacial side reactions during long-term cycling. Herein, a LiTaO 3 coating and Ta 5+ doping strategy are simultaneously achieved by a simple solid-phase synthesis. The surface side-reaction and undesired phase transition of LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA) are effectively restrained by this approach, which utilizes residual lithium to afford the coating. The NCA-LTO 3 (The modified NCA with a LiTaO 3 coating content of 3 wt%) delivers a high reversible capacity of 168.04 at 5 C (140.56 mAh g −1 for NCA), revealing the enhanced rate capability. More importantly, the cycling life could be greatly maintained after 200 cycles with a significant capacity retention of 94.1% (61.2% for NCA) at 1 C. Mechanism analysis indicates that such improvement is ascribed to the coating of conductor LiTaO 3 and doping Ta 5+ greatly promoting the Li-ion diffusion and stabilizing the interface of NCA. The study proposes a highly convenient strategy for interfacial optimization of cathode materials toward assisting the large-scale production of high-performance NCA.
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
Materials Today
·
2025
·
IF 22
Hong Zhang,Ao Zeng,Zhigang Zhang,Hua He,Yanwu Zhai,Tao He,Zhenbang Xu,Yoshihiro Kuroiwa,Sangwook Kim,Enyue Zhao,Xiaoling Xiao
High-voltage Ni-rich cathodes, which show high energy density and large cost-effectiveness, hold great promise for power Li-ion batteries. However, the unstable cyclic structure rooted in stress restricts their practical applications. In this work, we propose a strategy using a dispersed Eu 2 O 3 buffer phase to mitigate the high-voltage cyclic stress . The optimized Ni-rich cathode shows excellent high-voltage thermal stability and practical long-term cycling stability. For the constructed 4.6 V full cell, a superior capacity retention of 92 % after 200 cycles is observed. The enhanced cyclic properties are ascribed to the mitigated stress, as revealed by multi-characterizations such as in-situ X-ray diffractions and finite element simulation. As expected, the mitigated stress well stabilizes the oxygen lattice and preserves the particle structures. More importantly, the approach is confirmed to be versatile in other high-voltage cathodes. Also, other available elements including La and Dy for the construction of buffer phases are outlooked.
研究领域:
材料科学
·
电化学
·
锂离子电池
·
能源存储
·
固态化学
·
纳米材料
·
结构稳定性
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Chemistry
·
2025
·
IF 6.7
Jean Pierre Mwizerwa,Chenlong Gao,Changyong Liu,Wenfei Lu,Menghao Yang,Jun Shen
Constructing a robust, highly Li-ion-conductive surface layer is an effective strategy to improve the interfacial stability of nickel-rich cathodes like LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 O 2 (NCM811). However, existing methods often fail to balance ion/electron conductivity with suppression of surface phase transformations, leading to poor rate capability, cycling stability, and energy density. This work introduces an in-situ solution-phase formed coating of Li 4 SiO 4 (LSO) that creates a continuous ion/electron-conductive network across NCM811 particles. This LSO enhances lithium-ion transport, builds a stable electrode/electrolyte interface, and alleviates mechanical stress during cycling. As a result, NCM811@LSO exhibits improved electrochemical performance, including reduced voltage decay and stable operation at high voltages. The LSO coating suppresses surface degradation, intergranular cracking, and parasitic reactions by shielding active sites and reducing direct electrolyte contact. It also mitigates electrode polarization and localized overcharging during long-term cycling. Full-cell tests using graphite and SiO/C anodes confirm high energy densities, reaching 765 Wh kg −1 in NCM811@LSO//graphite cells. Furthermore, density functional theory (DFT) calculations support the experimental findings, revealing that LSO promotes favorable interfacial chemistry, suppresses internal cracking, inhibits nickel migration, and prevents irreversible phase transformations. Compared to traditional coatings, the multifunctional LSO layer offers superior protection and conductivity, making it a promising approach for developing advanced, high-energy-density lithium-ion batteries.
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Materials
·
2021
·Vol. 5
·期 4
·1294-1302
·
IF 15.122
Mengmin Jia,Chi Zhang,Yawei Guo,Linshan Peng,Xiaoyan Zhang,Weiwei Qian,Lan Zhang,Suojiang Zhang
The key to realize long-life high energy density lithium batteries is to exploit functional electrolytes capable of stabilizing both high voltage cathode and lithium anode. The emergence of localized high-concentration electrolytes (LHCEs) shows great promise for ameliorating the above-mentioned interfacial issues. In this work, a lithium difluoro(oxalate)borate (LiDFOB) based nonflammable dual-anion LHCE is designed and prepared. Dissolving in the mixture of trimethyl phosphate (TMP) /1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether (D 2 ), the continuously consumption of LiDFOB is suppressed by simply introducing lithium nitrate (LiNO 3 ). Meantime, as most of the TMP molecular are coordinated with Li + , the electrolyte does not show incompatibility issue between neither metal lithium nor graphite anode. Therefore, it demonstrates excellent capability in stabilizing the interface of Ni-rich cathode and regulating lithium deposition morphology. The Li||LiNi 0.87 Co 0.08 Mn 0.05 O 2 (NCM87) batteries exhibit high capacity retention of more than 90% after 200 cycles even under the high cutoff voltage of 4.5 V, 1 C rate. This study offers a prospective method to develop safe electrolytes suitable for high voltage applications, thus providing higher energy densities.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Lingjun Li,Lingfeng Xia,Huiping Yang,Xuehui Zhan,Jie Chen,Zhaoyong Chen,Junfei Duan
The high voltage application of the LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode is still hindered by its unstable surficial structure and poor capacity retention. Surface coating has been proved to be an effective strategy to deal with these problems. However, previous multistep surface coating approaches greatly complicate the synthesis procedure. In this work, a simple and large-scale solid-state approach is developed to prepare lanthanum-based oxides co-coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode materials . Electrochemical tests indicate that the co-coated samples exhibit superior cycle life and higher rate performance than those of the pristine sample. Further studies reveal that the enhanced interface stability and facilitated electron transportation can be attributed to the synergetic contribution provided by the lanthanum-based oxides co-coating layer. The present work demonstrates that our approach can achieve cathode synthesis and surface coating synchronously, and shows great potential to apply on a large scale and extent to all Ni-rich cathodes.
研究领域:
材料科学
·
电化学
·
能源存储
·
无机化学
·
功能材料
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）