ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qi Li,Xiaoyu Zhang,Jian Peng,Zhihao Wang,Zhixiang Rao,Yuyu Li,Zhen Li,Chun Fang,Jiantao Han,Yunhui Huang
Poly(ethylene oxide) (PEO)-based polymer electrolytes have been widely studied as a result of their flexibility, excellent interface contact, and high compatibility with a lithium metal anode. Owing to the poor oxidation resistance of ethers, however, the PEO-based electrolytes are only compatible with low-voltage cathodes, which limits their energy density. Here, a high-voltage stable solid-state interface layer based on polyfluoroalkyl acrylate was constructed via in situ solvent-free bulk electropolymerization between the LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode and the PEO-based solid polymer electrolyte. The electrochemical oxidation window of the as-synthesized electrolyte was therefore expanded from 4.3 V for the PEO-based matrix electrolyte to 5.1 V, and the ionic conductivity was improved to 1.02 × 10–4 S cm–1 at ambient temperature and 4.72 × 10–4 S cm–1 at 60 °C as a result of the improved Li+ migration. This fabrication process for the interface buffer layer by an in situ electrochemical process provides an innovative and universal interface engineering strategy for high-performance and high-energy-density solid-state batteries, which has not been explicitly discussed before, paving the way toward the large-scale production of the next generation of solid-state lithium batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
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电池技术
·
高分子化学
·
界面科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhen Sun,Yanqing Lai,Na lv,Yaqi Hu,Bingqin Li,Liangxing Jiang,Jiong Wang,Shuo Yin,Kui Li,Fangyang Liu
Argyrodite sulfide solid electrolytes, such as Li6PS5Cl (LPSC), have received much attention due to their high ionic conductivity (>1 mS cm–1) and success in all-solid-state batteries (long cycle performance, high energy density, etc.). Numerous efforts are spent on modifying the properties of the electrolyte itself. Here, we combine first-principles calculations with experiments to investigate O-doped argyrodite sulfide solid electrolytes (Li6PS5–xClOx,x = 0–1). It is found that Li6PS4.75ClO0.25 (LPSCO0.25) with x = 0.25 and cubic phase (F4̅3 m) shows the highest ion conductivity of 4.7 mS cm–1 (cold-pressed), higher than that of undoped Li6PS5Cl (4.2 mS cm–1). The bare LiCoO2/LPSCO0.25/Li–In all-solid-state battery exhibits an initial capacity of 131 mA h g–1 at 0.1 C and satisfactory cycling stability with 86% capacity retention after 250 cycles to the 4th cycle at 0.3 C under 25 °C. In addition, the NCM811/LPSCO0.25/Li–In cell is assembled using bare LiNi0.83Co0.06Mn0.11O2 cathode and shows an initial discharge capacity of 181 mA h g–1 at 0.1 C and 160 mA h g–1 at 0.3 C. The doping of oxygen-forming Li6PS5–xClOx also improves the stability to Li metal, proven by cyclic voltammetry and powder X-ray diffraction tests. The calculation results for the band structure reveals that LPSC has the lowest unoccupied molecular orbital than LPSCO0.25, further confirming the above conclusion.
研究领域:
材料科学
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电化学
·
能量存储
✓ 已验证
DOI
高影响因子
MATERIALS LETTERS
·
2025
·
IF 2.7
Caili He,Jinying Guo,Zhen Guo,Mengqi Ding,Hao Tang,Renjie Wang,Meifang Zhang
Layered oxide LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) is one of the promising cathode materials for high energy lithium ion batteries , which offering enhanced energy density and battery capacity. However, as the reaction progresses, a series of adverse effects arises. In this paper, the dual-additive electrolyte synergistic effect are ingeniously introduced to the traditional electrolyte LiPF 6 to form a low impedance and stable cathode electrolyte interface on the cathode surface. The specific discharge capacity of the battery at 5C was 154 mAh g −1 , while of the base electrolyte was only 106 mAh g −1 . The battery demonstrated over 82 % capacity retention after 200 cycles at 1C, while the base electrolyte was only 62 %.
研究领域:
电化学
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材料科学
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能源存储
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锂离子电池
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电极界面
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电解液工程
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2025
·Vol. 18
·期 9
·4362-4372
·
IF 30.8
Shengyao Luo,Mengqi Wu,Said Amzil,Tonghui Xu,Qing Ming,Lei Zhang,Jie Gao,Shuang Tian,Donghai Wang,Yisen Qian,Ya-Jun Cheng,Yonggao Xia
The combination of high-nickel cathodes with lithium metal anodes is widely considered a promising solution to alleviate range anxiety. However, challenges such as limited fast-charging capacity and rapid degradation persist when using carbonate-based electrolytes. While many researchers predominantly focus on solvation structures, we have strategically tailored the electrolyte formulation by employing isopropyl acetate as the primary solvent, evidenced by interfacial interactions. Compared to n-propyl acetate, isopropyl acetate reduced the interaction with the electrode surface, promoted tighter adsorption of the electrolyte ion network within the inner Helmholtz layer, and ultimately enhanced the dynamic stability of the lithium metal interface. In Li‖NCM811 cells, this electrolyte demonstrates a 4.5 V cutoff and sustains 88.6% capacity retention over 200 cycles at a high rate of 15C. Additionally, this electrolyte demonstrates stable cycling performance at elevated rates of 1C and 5C at temperatures of 60 °C and −20 °C, respectively, while maintaining stability even at a rate of 10C under poor electrolyte conditions with thin lithium layers, indicating significant application potential. These studies reveal that the electrolyte distribution at the electrode interface affects the electrochemical process and the formation of the electrode–electrolyte interphase significantly, offering new ideas for future electrolyte research and design.
研究领域:
电化学
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储能技术
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材料科学
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电池技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Huajun Zhao,Yunxian Qian,Guangfu Luo,Jian Chang,Chaoyang Wang,Jun Wang,Huaiyu Shao,Yonghong Deng
LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode coupling with artificial graphite (AG) is a promising tendency for high-energy-density batteries . However, realization of long-term lifespan under current realistic conditions remains a “Gordian knot” for large-scale commercialization-oriented realm owing to the aggressive and highly reactive Ni 4+ sites on the delithiated cathodes and electrolyte exhaustion. Vinylene carbonate (VC) is commonly employed as the additive for graphite anode in carbonate electrolytes. However, VC has limited protection ability for NCM811/AG, especially for high-temperature cycling, showing conspicuous gas generation and large interfacial resistance . Herein, advanced carbonate-based electrolytes containing vinylene carbonate (VC) and phosphate compounds like triallyl phosphate (TPPC2) and tripropargyl phosphate (TPPC3) as electrolyte additives are reported to improve the performance of NCM811/AG pouch cells at elevated temperature. Theoretical calculations and comprehensive characterizations reveal that these two electrolytes well regulate the electrodes interface with more robust and homogenous films. Moreover, the TPPC2 and TPPC3 additives exhibit stronger tendency to eliminate the corrosive active oxygen ( 1 O 2 ) released from NCM811. These merits mitigate the electrolyte decomposition, decrease the gas generation, inhibit the dissolution of transition metals from cathode, and protect the structure stability of NCM811. Such outstanding electrochemical performance reveals promising prospects in the commercialized application of NCM811/AG batteries .
研究领域:
电化学
·
材料科学
·
能源存储
·
锂离子电池
·
界面化学
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电极材料
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电解质工程
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 24
·2214274
·
IF 19
Shenghao Jing,Huaqing Shen,Yuting Huang,Wuqi Kuang,Zongliang Zhang,Siliang Liu,Shuo Yin,Yanqing Lai,Fangyang Liu
Sulfide-based all-solid-state batteries (ASSBs) have a wide application prospect because of the advantages of higher energy density and better intrinsic safety over conventional lithium-ion batteries (LIBs). The compatibility of sulfide-based electrolytes with various organic solvents and the possibilities of the slurry coating process with these systems remain veiled that limits the large-scale fabrication of sulfide-based ASSBs. In this study, polyvinylidene fluoride (PVDF) binder and isobutyl isobutyrate (IBB) are selected as the combination of binder and solvent to achieve scalable slurry process after examining the chemical and electrochemical compatibility of Li 6 PS 5 Cl (LPSC) solid electrolyte, PVDF, and IBB. A comparative investigation of sheet-type LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) electrodes and pellet-type NCM811 electrodes shows that PVDF hinders the transport of Li + and electron, but it benignantly works as a buffer layer, which alleviates the side reaction in the composite cathode electrode. Further, PVDF is modified by LiClO 4 to facilitate interfacial Li + transport, which improves the capacity retention of the cell at 0.5 C to 97.05% after 100 cycles. Finally, NCM811/graphite full-cell is successfully fabricated by the slurry coating process, which demonstrates the feasibility of practical and scalable fabrication of sulfide-based ASSBs with slurry process and its performance enhancement effect via LiClO 4 modification.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Xiaodong Bai,Chaoliang Zheng,Heng Zhang,Jian Liu,Panpan Wang,Baojia Xia,Jianling Li
PEO-based all-solid-state electrolytes are extensively utilized and researched owing to their exceptional safety, low-mass-density, and cost-effectiveness. However, the low oxidation potential of PEO makes the interface problem with the high-voltage cathode extremely severe. In this work, the impedance of PEO-based all-solid-state batteries with high-voltage cathode (NCM811) was studied at different potentials. The Nyquist plots displayed a gyrate arc at low-frequencies for NCM811/PEO interface. Based on the kinetic modeling, it was deduced that there is a decomposition reaction of PEO-matrix in addition to de-embedded reaction of NCM811, and the PEO intermediate product (dehydra-PEO) adsorbed on the electrode surface leading to low-frequency inductive arcs. Furthermore, the distribution of relaxation time shows the dehydra-PEO results in the kinetic tardiness of the charge transfer process in the temporal dimension. Hence, an artificial interface layer (CEI x ) was modified on the surface of NCM811 to regulate the potential of cathode/electrolyte interface to prevent the high-voltage deterioration of PEO. NCM/CEI x /PEO batteries exhibit capacity retentions of 96.0%, 84.6%, and 76.8% after undergoing 100 cycles at cut-off voltages of 4.1, 4.2, and 4.3 V, respectively. Therefore, here the failure mechanism of high-voltage PEO electrolyte is investigated by EIS and a proposed solving strategy is presented.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 22
·2426053
·
IF 19
Qixiang Jia,Zhujun Yao,Jiayuan Xiang,Juntao Shi,Yan Zhou,Jianhao Huang,Hongliang Zhang,Xiaoxiao Zhang,Yefeng Yang,Jiangping Tu
Li 2 ZrCl 6 (LZC) solid electrolyte has been recognized as a promising candidate for all-solid-state batteries (ASSBs), owing to its remarkable compatibility with high-voltage cathodes and the cost advantage among halide electrolytes. However, the ionic conductivity of LZC (≈0.4 mS cm −1 ) requires enhancement. Herein, rare earth metal elements (La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Yb, Y) have been doped into LZC, resulting in a doubling of the ionic conductivity. Moreover, Ta 5+ is utilized to further modulate the concentration of Li + to enhance the ionic conductivity and reduce the dosage of expensive rare-earth metal. Using the Li-Zr-Dy-Cl component as a case study, 16 types of Dy 3+ and Ta 5+ co-doped electrolytes have been synthesized and the optimal Li 2.1 Zr 0.8 Dy 0.15 Ta 0.05 Cl 6 (LZDTC) exhibits the ionic conductivity of 1.67 mS cm −1 . Three-dimensional Li-ion transport pathways in LZDTC has been revealed. The dual-substitution of Dy and Ta at Zr site changes length of Li-Cl bond and Li occupation, thereby reducing the resistance to Li + migration. ASSBs of Li-In/LGPS-LZDTC/NCM811 demonstrate a capacity of 117 mA h g −1 after 500 cycle at 0.5 C with a 74% retention rate, highlighting the effectiveness of the dual-doping strategy for creating superionic conductors for ASSBs.
研究领域:
材料科学
·
电化学
·
储能技术
·
固体离子学
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
Energy Advances
·
2022
·Vol. 1
·期 12
·1028-1034
·
IF 0
Lei He,Jian-Hua Cao,Ya-Kun Wang,Da-Yong Wu
Increasing the proportion of inorganic electrolytes in organic–inorganic composite electrolytes can significantly improve the ionic conductivity of composite electrolytes. However, this method is confronted with some problems, such as the uneven dispersion of inorganic electrolytes and the aggregation of nanoparticles, which results in a worse performance of the electrolytes’ interface. In this study, we had the dopamine hydrochloride molecules self-polymerized on the surface of inorganic ionic conductor lithium titanium aluminum phosphate (LATP) particles to obtain PDA-coated LATP nanoparticles. Then, the coated LATP particles were composited with PEO at a ratio of 80 : 20, with the LATP's evenly dispersed in the PEO, and no aggregation happened. On adding a small amount of electrolyte (5 μL cm−2, 1 M Li TFSI), the ionic conductivity of the electrospun PI-loaded PEO0.2–PDA@LATP0.8 flexible composite solid electrolyte reached 2.07 × 10−4 at 30 °C and 2.05 × 10−3 S cm−1 at 80 °C. NCM811‖Li batteries assembled with this electrolyte had an initial discharge capacity of 178.0 mA h g−1 at 30 °C, and still remained at 172.1 mA h g−1 (96.7%) after 200 cycles. The research shows that there are three main conduction pathways of Li+ in this electrolyte: through the segments of the polymer chains, through the interface between the polymer and inorganic ionic conductor, and through the passage composed of a continuous inorganic ionic conductor. Further results show that the coating of LATP by PDA does not block the transmission of Li+ both inside the crystal and at the crystal interface of LATP.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Jie Zhao,Saifang Huang,Yuyan Zhao,Bing Wu,Haiqin Lin,Zixuan Chen,Yudong Zhang,Weiji Dai,Can Cui
Solid-state lithium metal batteries (SSLMBs) face critical challenges, including low ionic conductivity, unstable electrode–electrolyte interfaces, and lithium dendrite growth issues. To address these issues, we designed a PVDF-based composite electrolyte embedded with NiSe nanosheets (PVDF-NS). The two-dimensional NiSe facilitated the in situ formation of Li2Se at the interface, promoting dendrite suppression by enhancing Li+ transport (room-temperature ionic conductivity: 5.53 × 10–4 S·cm–1; transference number: 0.449) and constructing a stable SEI layer. Notably, PVDF-NS supported Li||Li symmetric cells demonstrated excellent stability for over 2000 h at 0.2 mA·cm–2. When paired with NCM811 cathodes, full cells demonstrated 86.3% capacity retention over 300 cycles at 2 C. Additionally, the electrolyte exhibited high oxidative stability (4.83 V vs Li+/Li) and retained a capacity of 65.6 mAh·g–1 at 5 C, underscoring its practical applicability. This interfacial engineering approach presents a scalable and effective route for developing durable, high-performance solid electrolytes for next-generation SSLMBs.
研究领域:
材料科学
·
电化学
·
储能
·
纳米技术
·
电池技术
✓ 已验证
产品关联
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
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2025
·Vol. 35
·期 7
·2341-2353
·
IF 4.7
Han-zhou LIU,Yan-chen LIU,Sheng-hao JING,Ya-qi HU,Zong-liang ZHANG,Si-liang LIU,Yang LIU,Zhi ZHUANG,Fan-qun LI,Fang-yang LIU
A dual-halide solid electrolyte, Li 3 YCl 3 Br 3 , was synthesized using a wet-chemistry route instead of the conventional mechanical ball-milling route. Li 3 YCl 3 B r3 exhibits an ion conductivity of 2.08 mS/cm and an electro- chemical stability window of 3.8 V. Additionally, an all-solid-state lithium-ion battery using Li 3 YCl 3 Br 3 and LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) as the cathode material achieves a capacity retention of 93% after 200 cycles at 0.3 C and maintains a specific capacity of 115 mA·h/g during 2 C cycling. This exceptional performance is attributed to the high oxidative stability of Li 3 YCl 3 Br 3 and the in-situ formation of Y 2 O 3 inert protective layer on the NCM811 surface under high voltage. Consequently, the study demonstrates the feasibility of a simple, cost-effective wet-chemistry route for synthesizing multi-component halides, highlighting its potential for large-scale production of halide solid electrolytes for practical applications.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源存储
·
电池技术
·
无机非金属材料
·
纳米材料应用
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）