Energy & Environmental Materials
·
2025
·
IF 14.1
Yuanxin Gao,Xinyi Wang,Dong Lv,Zhang Zhang,Jiangpeng Li,Xiaoyan Feng,Jingchao Chai,Yun Zheng,Yu Peng,Yanqing Wang,Yingying Wang,Lingyu Zhu,Zhihong Liu
Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10 −4 S cm −1 ) and anodic stability (>4.4 V vs Li + /Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li + transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.
研究领域:
电化学
·
材料科学
·
能源化学
·
界面化学
·
锂离子电池
·
电极材料
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2020
·Vol. 8
·期 2
·2001809
·
IF 15.84
Ze Feng,Ranjusha Rajagopalan,Shan Zhang,Dan Sun,Yougen Tang,Yu Ren,Haiyan Wang
LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes suffer from severe bulk structural and interfacial degradation during battery operation. To address these issues, a three in one strategy using ZrB 2 as the dopant is proposed for constructing a stable Ni-rich cathode. In this strategy, Zr and B are doped into the bulk of LiNi 0.8 Co 0.1 Mn 0.1 O 2 , respectively, which is beneficial to stabilize the crystal structure and mitigate the microcracks. Meanwhile, during the high-temperature calcination, some of the remaining Zr at the surface combined with the surface lithium source to form lithium zirconium coatings, which physically protect the surface and suppress the interfacial phase transition upon cycling. Thus, the 0.2 mol% ZrB 2 -LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode delivers a discharge capacity of 183.1 mAh g −1 after 100 cycles at 50 °C (1C, 3.0–4.3 V), with an outstanding capacity retention of 88.1%. The cycling stability improvement is more obvious when the cut-off voltage increased to 4.4 V. Density functional theory confirms that the superior structural stability and excellent thermal stability are attributed to the higher exchange energy of Li/Ni exchange and the higher formation energy of oxygen vacancies by ZrB 2 doping. The present work offers a three in one strategy to simultaneously stabilize the crystal structure and surface for the Ni-rich cathode via a facile preparation process.
研究领域:
材料科学
·
电化学
·
储能
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Qingmeng Gan,Ning Qin,Youhuan Zhu,Zixuan Huang,Fangchang Zhang,Shuai Gu,Jiwei Xie,Kaili Zhang,Li Lu,Zhouguang Lu
The Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode has attracted great interest owing to its low cost, high capacity, and energy density. Nevertheless, rapid capacity fading is a critical problem because of direct contact of NCM811 with electrolytes and hence restrains its wide applications. To prevent the direct contact, the surface inert layer coating becomes a feasible strategy to tackle this problem. However, to achieve a homogeneous surface coating is very challenging. Considering the bonding effect between NCM811, polyvinylpyrrolidone (PVP), and polyaniline (PANI), in this work, we use PVP as an inductive agent to controllably coat a uniform conductive PANI layer on NCM811 (NCM811@PANI–PVP). The coated PANI layer not only serves as a rapid channel for electron conduction, but also prohibits direct contact of the electrode with the electrolyte to effectively hinder side reaction. NCM811@PANI–PVP thus exhibits excellent cyclability (88.7% after 100 cycles at 200 mA g–1) and great rate performance (152 mA h g–1 at 1000 mA g–1). In situ X-ray diffraction and in situ Raman are performed to investigate the charge–discharge mechanism and the cyclability of NCM811@PANI–PVP upon electrochemical reaction. This surfactant-modulated surface uniform coating strategy offers a new modification approach to stabilize Ni-rich cathode materials for lithium-ion batteries.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Chemistry
·
2023
·
IF 7.3
X. Dong,L. Dou,A. Tang,P. Hu,Z. Zhang,C. Shang
LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), as a promising Ni-rich electrode material for lithium-ion batteries, is hindered by the interface instability and structure degradation caused by electrolyte erosion during operation. In this work, with the addition of thiophene into traditional electrolyte, the elastic conductive polythiophene (PTh) is in-situ electrochemically polymerized on the surface of NCM811 to stabilize the interface and hinder electrolyte corrosion. As expected, the PTh-modified NCM811 shows improved cycling stability at 2 C with capacity retention of 94% after 200 cycles and considerable rate capability with high specific capacity of 171.7 mAh/g at 5 C. This work provides an effective and feasible method to employ conductive polymer as elastic protective layer for electrode 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
Materials
·
2023
·Vol. 16
·期 10
·3613
·
IF 3.4
Fu Long,Yuyang Liu,Guobin Zhu,Yan Wang,Honghe Zheng
The application of nickel-rich cathodes in lithium-ion batteries has been hampered by its rapid capacity/voltage fading and limited performance of rate. In this work, a passivation technique is used to create a stable composite interface on single-crystal LiNi0.8Co0.1Mn0.1O2(NCM811) surface, which greatly improves the cycle life-span and high-voltage constancy of cathode with 4.5 and 4.6 V cut-off voltage. The improved Li+conductivity of the interface enables a firm cathode–electrolyte interphase (CEI), which reduces interfacial side reactions, lowers the risk of safety hazards, and improves irreversible phase transitions. As a result, the electrochemical performance of single-crystal Ni-rich cathode are remarkably enhanced. The specific capacity of 152 mAh g−1can be delivered at a charging/discharging rate of 5 C under 4.5 V cut-off voltage, much higher than 115 mAh g−1of the pristine NCM811. After 200 cycles at 1 C, the composite interface modified NCM811 demonstrates outstanding capacity retention of 85.4% and 83.8% at 4.5 V and 4.6 V cut-off voltage, respectively.
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
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 8
·4494-4504
·
IF 11.301
Song-Yi Liao,Xing-Wen Huang,Qiu-Shi Rao,Yue-Zhu Li,Jun-Qi Hu,Feng Zheng,Zhi-Yuan Ma,Ting-Ting Cui,Yi-Dong Liu,Yong-Gang Min
LiNi0.8Co0.1Mn0.1O2 (NCM811) has attracted increasing attention owing to its extremely high discharge capacity (>200 mA h g−1). However, poor mechanical strength, cycling stability, and rate capability impose limitations on its large-scale practical applications. Here, we report that few-layer and rod-like MXene (Ti2C3Tx) as a multifunctional additive significantly enhances the mechanical property, cycling performance, and rate capability of the Li/NCM811 cells. Thus, NCM811 added with 2.5 wt% MXene (2.5-MXene) delivers the highest discharge capacity of 209 mA h g−1 at 0.2C as well as the best rate performance with a high reversible capacity of 95 mA h g−1 at 8C. Moreover, the capacity retention of 2.5-MXene can reach 77.0% after 100 cycles at a 0.5C rate, while it is only 53.6% for pristine NCM811 without MXene (0-MXene). Such superior performances result from the effective and multifunctional MXene additive, which is helpful to establish a better conductive network, store/release Li+via cation intercalation, offer more deformation space, form a physical protection CEI layer, and suppress the M ↔ H2 phase transformation for the NCM811 electrodes. In addition, the DFT calculation indicates that the MXene additive can prohibit the irreversible Ni/Co/Mn elements' migration via the absorption process. Therefore, the few-layer/rod-like MXene can be a facile and efficient approach to enhance the mechanical and electrochemical performance of the NCM811 materials for large-scale applications in the next-generation energy density lithium-ion batteries by considering its multifunctional properties, low cost, and convenient accessibility.
研究领域:
材料科学
·
能源存储
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Tao Jiang,Bowen Zhu,Haiyun Shen,Ying Liu,Hao Liu,Wei Zheng,Mengtao Wu,Ning Xu,Li Chen
The Ni-rich LiNixCoyMn1–x–yO2 with high specific capacity and superior thermal stability under a high cutoff voltage (>4.3 V) will play a critical role in high-power lithium-ion batteries (LIBs). In this paper, LiNi0.8Co0.1Mn0.1O2 (NCM811) equipped with a stable garnet ceramic Li6.5La3Zr1.5Ta0.5O12 (LLZTO) nanoshell is successfully synthesized via a simple wet chemical approach. X-ray diffraction, scanning electron microscope (SEM), energy-dispersive spectrometer (EDS) element mapping, and transmission electron microscopy (TEM) confirm the presence of LLZTO on the NCM811 surface. The NCM811 with 2 wt % LLZTO (2-NCM811) can deliver a superior specific capacity of 144.4 mAh·g–1 at 1C (2.8–4.3 V) after 100 cycles, accompanied by a capacity retention rate as high as 81.1%. But pristine NCM811 has a discharge capacity of only 119.6 mAh·g–1 and a capacity retention rate as low as 69.5% under the same condition. What is more, 2-NCM811 exhibits an enhanced discharge capacity of 129.6 mAh·g–1 at 1C (2.8–4.5 V) after 100 cycles and a high capacity retention rate of 62.9%, which are superior to those of pristine NCM811 (110.0 mAh·g–1, 57.6%). The improved high-potential performance of 2-NCM811 can be attributed to the positive role of the LLZTO shell, which enhances the structural stability and simultaneously inhibits adverse side reactions at the surface of 2-NCM811 during cycling. Based on the above advantages, LLZTO with three-dimensional (3D) diffusion pathways and high ion conductivity is expected to be the most prospective material for the surface modification engineering of nickel-rich cathode materials in lithium-ion batteries (LIBs).
研究领域:
材料科学
·
电化学
·
储能技术
·
锂离子电池
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 36
·20633-20639
·
IF 10.733
Huilin Xie,Chunli Li,Wang Hay Kan,Maxim Avdeev,Chenyou Zhu,Zhikun Zhao,Xiaorong Chu,Daobin Mu,Feng Wu
All solid-state batteries have received significant attention due to their excellent safety performance. As a key component, the garnet-type electrolyte is one of the best known electrolytes due to its air stability and good compatibility with metallic lithium. However, the total Li+ conductivity of this kind of electrolyte is usually lower than that of the bulk electrolyte primarily due to the grain boundary resistance. In this study, we focused on engineering the electrolyte Li6.4La3Zr1.4Ta0.6O12 (LLZTO) by introducing Li3BO3 (LBO) into it to form the electrolyte LLZTO/LBO with the aim to consolidate the grain boundary. Via characterization by both neutron and X-ray diffraction, the as-prepared LLZTO was indexed as a pure cubic phase, where Ta certainly substituted the Zr sites. LLZTO/LBO still maintained the cubic structure, and the B atoms did not occupy any cation sites in the unit cell. It was demonstrated that an amorphous phase of a boracic substance was trapped inside the cubic LLZTO phase. The amorphous boracic phase sutured the gaps among the LLZTO grains and then lowered the grain boundary resistance without introducing impurities, ultimately consolidating the solid-state electrolyte. Electrochemical impedance spectroscopy revealed that the total Li+ conductivity of LLZTO/LBO reached 5.47 × 10−4 S cm−1, much higher than those of the as-prepared Li7La3Zr2O12 (LLZO) and LLZTO. Using LLZTO/LBO as an electrolyte, the LiNi0.8Co0.1Mn0.1O2/LiFePO4 hybrid solid battery showed an excellent cycling performance with the reversible capacity of 147.8 mA h g−1 at 0.2C for 100 cycles and the capacity retention of 93.8%. These results suggest that the consolidation of the grain boundary with LBO is a promising way to achieve an improved electrolyte, LLZO, with higher total Li+ conductivity.
研究领域:
材料科学
·
电化学
·
储能技术
·
固态电池
✓ 已验证
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Hongzhi Wang,Yi Bo Shang,Weiguo Zhang,Fei Ding,Lin Sang
In recent years, the rapid development of the electric vehicle industry has led to the requirement of Li-ion batteries (LIBs) with a higher energy density and better safety. Therefore, solid-state lithium batteries with the above advantages have attracted a lot of attention. However, solving the interfacial problem between cathodes and the solid-state electrolyte has become a major challenge in the practical application of solid-state lithium-ion batteries. In this article, ETPTA (trimethylolpropane ethoxylate triacrylate)-PEG (poly(ethylene glycol)) is introduced onto the surface of LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 O 2 cathode materials by ultraviolet irradiation. TEM and FTIR analyses reflect the existence of the composite coating layer. Electrochemical tests reveal that the coated material has better cycle stability (capacity retention remains 84% after 100 cycles), lower interfacial impedance and higher rate capabilities (34 mA h g -1 at 2 C). These results reflect the fact that the coating layer plays a significant role in improving the interfacial contact between the cathode and solid-state electrolyte and suppressing surface side reactions.
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
Nature Energy
·
2023
·Vol. 8
·期 8
·800-813
·
IF 56.7
Yan Wenlin,Mu Zhenliang,Wang Zhixuan,Huang Yuli,Wu Dengxu,Lu Pushun,Lu Jiaze,Xu Jieru,Wu Yujing,Ma Tenghuan,Yang Ming,Zhu Xiang,Xia Yu,Shi Shaochen,Chen Liquan,Li Hong,Wu Fan
All-solid-state batteries (ASSBs) with Li metal anodes or Si anodes are promising candidates to achieve high energy density and improved safety, but they suffer from undesirable lithium dendrite growth or huge volume expansion, respectively. Here we synthesize a hard-carbon-stabilized Li–Si alloy anode in which sintering of Si leads to the transformation of micro-metre particles into dense continuum. A 3D ionic-electronic-conductive network composed of plastically deformable Li-rich phases (Li 15 Si 4 and LiC 6 ) that enlarges active area and relieves stress concentration is created in the anode, leading to improved electrode kinetics and mechanical stability. With the hard-carbon-stabilized Li-Si anode, full cells using LiCoO 2 or LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes and Li 6 PS 5 Cl electrolyte achieve favourable rate capability and cycle stability. In particular, the ASSB with LiNi 0.8 Co 0.1 Mn 0.1 O 2 at high loading of 5.86 mAh cm −2 delivers 5,000 cycles at 1 C (5.86 mA cm −2 ), demonstrating the potential of using hard-carbon-stabilized Li–Si alloy anodes for practical applications of ASSBs.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Wu,Zhenyao Wei,Jun Wang,Jian Shang,Man Wang,Shang-Sen Chi,Qingrong Wang,Leilei Du,Tian Zhang,Zijian Zheng,Yonghong Deng
Flexible solid-state batteries (FSSBs) are indispensable energy storage devices to fulfil the energy and safety requirements for future flexible applications. The bottlenecks of FSSBs are how to realize high energy density with competent ionic conductivity for room-temperature (RT) flexible applications. Here, the first fabrication of RT FSSB with high energy density is reported, which is realized by in situ integration of a 20-µm-thick hybrid polymer/ceramic/ionic liquid solid-state electrolyte (SSE) between the high energy combination of anode/cathode electrodes. The in situ electrode/electrolyte interfacial integration strategy provides an ultrathin SSE layer, ultralow resistance and superior flexibility, and the SSE guarantees both high ionic conductivity and good compatibility with high-energy cathode LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811). The fabricated Li 4 Ti 5 O 12 /NCM811 FSSB delivers super-low resistance approaching conventional liquid cells and excellent cycling stability up to 600 cycles at RT. The extension of anode to SiO x @graphite leads to a high theoretical energy density of 489.6 Wh kg −1 at material’s level, times higher than current options. In addition, the RT FSSB shows great flexibility, indicating a high performance application in future flexible electronics.
研究领域:
能源存储
·
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 40
·2401204
·
IF 13
Siyu Fang,Chengyu Han,Shaojie Zhang,Yu Cao,Kang Ma,Yiming Zhang,Xinpeng Han,Juan Wang,Jie Sun
The demand for state-of-the-art high-energy-density lithium-ion batteries is increasing. However, the low specific capacity of electrode materials in conventional full-cell systems cannot meet the requirements. Ni-rich layered oxide cathodes such as Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 (NCM811) have a high theoretical specific capacity of 200 mAh g −1 , but it is always accompanied by side reactions on the electrode/electrolyte interface. Phosphorus anode possesses a high theoretical specific capacity of 2596 mAh g −1 , but it has a huge volume expansion (≈300%). Herein, a highly compatible and secure electrolyte is reported via introducing an additive with a narrow electrochemical window, Lithium difluoro(oxalato)borate (LiDFOB), into 1 m LiPF 6 EC/DMC with tris (2,2,2-trifluoroethyl) phosphate (TFEP) as a cosolvent. LiDFOB participates in the formation of organic/inorganic hybrid electrode/electrolyte interface layers at both the cathode and anode sides. The side reactions on the surface of the NCM811 cathode and the volume expansion of the phosphorus anode are effectively alleviated. The NCM811//RP full cell in this electrolyte shows high capacity retention of 82% after 150 cycles at a 0.5C rate. Meanwhile, the electrolyte shows non-flammability. This work highlights the importance of manipulating the electrode/electrolyte interface layers for the design of lithium-ion batteries with high energy density.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）