ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yu Peng,Jiawei Chen,Gaopan Liu,Yue Yin,Xiaoli Fang,Yonggang Wang,Xiaoli Dong,Yongyao Xia
Lithium metal batteries (LMBs) with Li metal anodes and high-voltage LiCoO 2 (LCO) cathodes offer high energy density but face challenges such as Li dendrite growth and LCO structure degradation, which primarily arises from the electrolyte's inability to form a stable interphase. Herein, a dual-additive optimized carbonate-based electrolyte is developed, incorporating tetraethylammonium nitrate (TEANO 3 ) and lithium difluorobis(oxalato) phosphate (LiDFBOP) as regulators. LiDFBOP enhances interfacial stability and compactness, while TEANO 3 facilitates Li + transport and suppresses excessive decomposition of LiDFBOP. The synergistic effect of TEANO 3 and LiDFBOP establishes robust, high ion-conductive solid electrolyte interphase (SEI) and cathode–electrolyte interphase (CEI) enriched with P- and N-containing inorganic compounds (including LiN x O y and P-O/P-F species), enabling dense Li deposition and stable cycling of LCO under a high cut-off voltage of 4.5 V. The optimized electrolyte enables Li||LCO full cells with a high capacity retention of 84% even with high-mass-loading LCO cathode (3.5 mAh cm −2 ) and limited Li (N/P = 2). This work demonstrates a straightforward electrolyte design strategy for optimizing SEI and CEI, advancing the practical deployment of LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
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
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Xiang Zhou,Dingding Zhu,Yong Su,Feixiang Wu,Xiaolei Ren,Xuedong Zhang,Xiangze Ou,Yaling Rao,Long Xie,Liang Tang,Jianyu Huang,Qiao Huang
Metal fluorides (MFs) are regarded as high-capacity conversion cathode materials for next-generation lithium-ion batteries with high energy density. However, these cathodes suffer from poor electronic conductivity, sluggish reaction kinetics, and deleterious cathode solid electrolyte interface (CEI) formation, which may cause rapid cell degradation upon cycling. Herein, a low temperature chemical vapor deposition (CVD) carbon coating technology is successfully achieved to coat MFs-FeF 2 with a thin amorphous carbon layer, which promotes the formation of a stable CEI with improved electronic and ionic transport property. Consequently, a discharge capacity higher than 450 mAh g −1 of the CVD coated FeF 2 is achieved with a capacity retention at about 75% after 2500 cycles in a saturated electrolyte. Moreover, an unprecedented cycling performance with the discharge capacity of 350 mAh g −1 after 500 cycles in a super diluted electrolyte is also achieved. Advanced cryo-electron microscopy reveals that the carbon coating significantly suppresses the undesirable CEI formation and promotes the formation of a thin CEI with excellent chemo-mechanical property. This work provides a feasible technology to stabilize the important interface on MFs and offers a new strategy to accelerate the commercial adoption of such 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
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 ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zerui Chen,Yingxinjie Wang,Jie Wang,Xiaohui Li,Guohao Li,Ziying Zhang,Zhenjun Wu,Xiuqiang Xie,Nan Zhang
Manganese-based Prussian blue analogues (PBA) have garnered widespread attention as the promising cathode materials for sodium-ion batteries. However, the inevitable Jahn-Teller distortion and the formation of unstable and uneven cathode electrolyte interphase (CEI) result in severe Mn dissolution and poor cycling stability. Herein, we report a simple MXene modification strategy cold pressing method to embed Prussian blue cathode materials into MXene nanosheets. This highly conductive protective barrier not only mitigates the Jahn-Teller distortion in Mn-PBA and maintains the integrity of the particles during charge–discharge cycles, but also partially suppresses side reactions between the electrolyte and cathode interface through surface functional groups (−F), resulting in a thin and uniform CEI. The protection of the stable CEI and MXene nanosheets simultaneously alleviate the Jahn-Teller effect and suppress the Mn dissolution during long cycling, thus allowing the cathode material to retain ∼ 80 % of its capacity after 1000 cycles at a current density of 1000 mA g −1 . This study highlights the importance of stabilizing the cathode interface and provides a novel approach for preparing highly stable manganese-based PBA cathode.
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
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Gaopan Liu,Ningbo Xu,Yue Zou,Ke Zhou,Xuerui Yang,Tianpeng Jiao,Wu Yang,Yong Yang,Jianming Zheng
Ni-rich layered structure materials are appealing cathodes for high-energy-density lithium-ion batteries developed for electric vehicles, drones, power tools, etc. However, poor interfacial stability between a Ni-rich cathode and carbonate electrolyte, especially at high temperatures, and fast capacity fading still hinder their mass market penetration. Here, we investigate cyclopentyl isocyanate (CPI) with a single isocyanate (−NCO) functional group as a bifunctional electrolyte additive for the first time to improve the interfacial stability of Ni-rich cathode LiNi0.83Co0.12Mn0.05O2 (NCM83). With an electrolyte containing 2 wt % CPI, the NCM83 cathode shows capacity retention of up to 92.3% after 200 cycles at 1C and 30 °C, much higher than that with the standard electrolyte (78.6%). It is demonstrated that the −NCO of CPI could largely inhibit the thermal decomposition of LiPF6 salt and scavenge water and hydrogen fluoride (HF) species, improving electrolyte stability. More importantly, the additive CPI could be preferentially oxidized, forming a stabilized and protective cathode electrolyte interphase (CEI) layer on the surface of NCM83, which effectively suppresses the parasitic side reactions and maintains the superior interfacial charge-transfer and lithium-ion diffusion kinetics. Both functions enable a significant improvement in electrochemical performance at both 30 and 60 °C.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Batteries & Supercaps
·
2023
·
IF 5.7
Pengfei Liu,Yuxin Rao,Huasong Wang,Xue Li,Xiaomin Wang,Miaomiao Yu,Yong Li,Zhihao Yue,Fanglin Wu,Shan Fang
Graphical Electrolyte cosolvent : We employed methyl (2,2,2-trifluoroethyl) carbonate (FEMC) as a co-solvent for the [LiTFSI] 3 [Pyr 14 FSI] 4 (ILE) to enhance the cycling stability cathode materials. Experimental results indicate that the introduction of FEMC can effectively form a LiF-rich cathode electrolyte interface (CEI) layer, which effectively suppress the cracking of secondary particles and contribute to enhance the performance of the high-mass loading of Li||LiFePO 4 (LFP) cells. Ionic liquids (ILs) are promising electrolyte candidates for high-safety and stability lithium metal batteries. However, their practical application is hindered by high viscosity resulting in a poor wettability of separator and sluggish Li + transport at room temperature. Herein, a weakly-solvating solvent of methyl (2,2,2-trifluoroethyl) carbonate (FEMC) is employed as a co-solvent in non-flammable ionic-liquid electrolyte (ILE) which composed with N-butyl-N-methylpyrrolidinium bis (fluorsulfonyl) imide (Pyr 14 FSI) and bis (trifluoromethanesulfonyl) sulfonimide lithium salt (LiTFSI), effectively ameliorates the shortcomings of ILs mentioned above without sacrificing its safety character. Compared with pure ILE, the addition of FEMC can distinctly decrease the polarization voltage and electrode-electrolyte interface resistance. With the assistance of FEMC solvent, the discharge specific capacity of Li||LiFePO 4 (LFP) and Li||LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cells are significantly improved. The origin of this great improvement is contributed to the exceptionally stable and LiF-rich cathode electrolyte interphase (CEI) layer formed in this electrolyte. Additionally, Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cells exhibit a remarkable rate capability (105 mAh g −1 at 2 C rate), achieve an initial specific capacity of 202.8 mAh g −1 and outstanding capacity retention of 88.2 % over 100 cycles.
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 Polymer Materials
·
2023
·
IF 5
Yutao Xu,Fatima Zahra Chafi,Peng Chen,Cancan Peng,Ya-Jun Cheng,Kunkun Guo,Xiuxia Zuo,Yonggao Xia
Nickel-rich layered cathodes (for example, NCM811) hold great promise for practical applications in high-energy density lithium-ion battery technology. However, a nickel-rich cathode has poor cyclic stability because of the structure degradation induced by repeated cycles and excessive formation of thick cathode–electrolyte interface (CEI) layers. Poly(vinylidene difluoride) (PVDF) is a typical binder used to form a positive electrode, which nevertheless lacks the functionality to suppress structure degradation and control CEI layer formation. A new concept is proposed in this work to use a multi-functional block copolymer of poly(ether imide)-block-poly(dimethyl siloxane) (PEI-b-PDMS; abbreviated as PEMS) as the binder for the nickel-rich cathode. Unlike the conventional PVDF binder, the PEMS binder is capable of inhibiting crack formation within the NCM811 particles to retard structure degradation over cycles because of its elastomeric feature. The PEMS binder also enables tuning the composition of the CEI layer and inhibits the formation of overly thick CEI layers because the carbonate solvent molecules are excluded from the solvation sheath by the PEMS binder. Enhanced electrolyte affinity is exhibited by the electrode with the PEMS binder as evidenced by the contact angle measurement. Improved carbon black dispersion within the electrode is achieved by the PEMS binder because the PEI aromatic chain has strong affinity toward the carbon black particles. Both the cycling and rate performance of the NCM811 cathode is improved with the PEMS binder compared to the PVDF binder. In detail, the capacity retention is increased from 63.9 to 80.6% after 200 cycles at 0.5 C (1 C = 205 mAh g–1) when the PVDF binder is replaced by the PEMS binder. The rate performance at current densities of 2 and 5 C is increased significantly due to enhanced electrochemical kinetics.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
eScience
·
2022
·
IF 0
Wei Gu,Guoyong Xue,Qingyu Dong,Ruowei Yi,Yayun Mao,Lei Zheng,Haikuo Zhang,Xiulin Fan,Yanbin Shen,Liwei Chen
Ni-rich layered oxides are attractive cathode materials for advanced lithium-ion batteries (LIBs) due to their high energy density. However, their large-scale application is seriously hindered by their interfacial instability, especially at a high cut-off potential. Here, we demonstrate that trimethoxyboroxine (TMOBX) is an effective film-forming additive to address the interfacial instability of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) material at a high cut-off voltage of 4.5 V. We find that TMOBX decomposes before carbonate solvent and forms a thin cathode electrolyte interphase (CEI) layer on the surface of the NCM811 material. This TMOBX-formed CEI significantly suppresses electrolyte decomposition at a high potential and inhibits the dissolution of transition metals from NCM811 during cycling. In addition, electron-deficient borate compounds coordinate with anions ( P F 6 − , F − , etc.) and H 2 O in the battery, further improving the battery's stability. As a result, adding 1.0 wt% of TMOBX boosts the capacity retention of a Li||NCM811 cell from 68.72% to 86.60% after 200 cycles at 0.5C in the range of 2.8–4.5 V.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
Advanced Energy Materials
·
2021
·Vol. 11
·期 39
·2101956
·
IF 29.368
Jixiang Yang,Xiang Liu,Yian Wang,Xinwei Zhou,Lutao Weng,Yuzi Liu,Yang Ren,Chen Zhao,Mouad Dahbi,Jones Alami,Deia Abd Ei-Hady,Gui-Liang Xu,Khalil Amine,Minhua Shao
Lithium-ion batteries (LIBs) based on LiNi x Co y Mn 1-x-y O 2 (NCM) cathode materials have been widely commercialized, because of their high energy density, favorable rate performance, and relatively low cost. However, with increased Ni content to further increase their energy density, their cycling stability deteriorates dramatically and thus fails to meet the commercial application requirements. The artificial cathode-electrolyte-interphase (CEI) is a promising approach to solve this problem. Here, a robust CEI is fabricated through in situ polymerization of ethylene carbonate induced by aluminum isopropoxide (AIP). By adding 1 wt.% AIP in a commercial electrolyte, the capacity retention of LiNi 0.8 Co 0.1 Mn 0.1 O 2 ||Li cell at 1 C rate has been significantly increased from 80.8% to 97.8% with a highly reversible capacity of 176 mA h g −1 after 200 cycles. AIP can be also used as an additive during the slurry-making process, enabling a reversible capacity of 170 mA h g −1 for LiCoO 2 after 200 cycles even at a high charge cut-off voltage of 4.6 V. It is confirmed that the in situ formed CEI layer can prevent the cathodes from cracking and reduce the irreversible phase transformation.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Xiaomei Zhang,Zheng Xu,Jian Xie,Yunhao Lu,Shuangyu Liu,Xiongwen Xu,Jian Tu,Bo Xu,Xinbing Zhao
Na-ion batteries are considered as promising battery systems for large-scale energy storage. Although Na-ion batteries exhibit enhanced low-temperature cycling performance compared with lithium-ion batteries, there is still a great challenge to overcome for practical low-temperature applications. In this work, we propose a low-performance Na-ion battery composed of FeNi co-doped Mn-based Prussian cathode (FeNi-MnHCF) and a low-concentration electrolyte (0.5 mol L −1 ) containing a small amount of 2,2,2-trifluoroethyl acetate (ETFA, 1 wt%). The introduction of ETFA could decrease the viscosity , increase ionic conductivity and change the solvation structure of the electrolyte at low temperature. ETFA could also participate in constructing a uniform, stable, and Na-ion conductive CEI layer, enabling rapid Na-ion transport and effective protection of FeNi-MnHCF. The cells with the ETFA-contained electrolyte and FeNi-MnHCF cathode exhibit excellent rate capability and long cycle life at low temperature. When being cycled at −20 °C, the cell with ETFA could retain 92.1 % of the capacity after 1120 cycles at 1 C. The cell could also show stable cycling after overcharge to 4.8 V or overdischarge to 1.2 V at −20 °C. This work sheds light on the design of long-life and robust Na-ion batteries for sustainable energy storage at low temperature.
研究领域:
材料科学
·
能源存储
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Peng Zhang,Jian-Hua Cao,Wei-Hua Liang,Yue Li,Ya-Kun Wang,Da-Yong Wu
Solid electrolytes are generated through in situ polymerization within batteries, which is one of the most promising methods for achieving solid-state lithium metal batteries with good interfacial contact, high safety, and high performance. Poly-1,3-dioxolane (PDOL), although a good in situ solidified electrolyte for lithium stability, has poor applicability in high-voltage battery systems. In order to improve the interfacial compatibility between PDOL and both the cathode and anode of high-voltage batteries. we herein design a sacrificial additive, diethyl (2,2,2-trifluoroethyl) phosphite (DETFPi), with a lower lowest unoccupied molecular orbital (LUMO) and higher highest occupied molecular orbital (HOMO) energy, through methods of calculation. After being loaded into the battery, DETFPi-DOL is in situ polymerized to form DETFPi-PDOL electrolyte. The Li||DETFPi-PDOL||Li symmetric battery operates stably for 2000 h at 0.5 mA cm–2, with an overpotential of only 16 mV. XPS analysis shows that an SEI layer with high LiF content is formed on the surface of the lithium anode after cycling, which promotes the uniform deposition of lithium ions and inhibits the growth of lithium dendrites. After 300 cycles, the NCM811||DETFPi-PDOL||Li battery exhibits a remaining capacity of 154.8 mAh g–1 (81%) within the 3.0–4.35 V range, meanwhile demonstrating excellent rate performance. Moreover, a uniform CEI layer containing pentavalent phosphorus and low LiF content is formed on the surface of the cathode after battery cycling. Finally, due to the improvement of the cathode interface, the increase of interfacial impedance of the battery after 300 cycles is reduced to half that of the PDOL battery.
研究领域:
材料科学
·
电化学
·
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）