Journal of Energy Storage
·
2024
·
IF 8.9
Wenjie Yuan,Jinlong Liao,Songde Huang,Dakun Song,Qinting Su,Cuihua Li,Jinhua He
Solid lithium metal batteries with solid polymer electrolytes have advantages in terms of high energy density and safety. However, their application is still hindered by unstable solid electrolyte interfaces (SEI and CEI) and uncontrolled dendrite growth. Here, a composite skeleton loaded with dielectric filler yttrium stabilized zirconia nanoparticles (YSZ) on the surface of PVDF-HFP nanofiber filaments is designed, and a novel composite solid electrolyte (CSE) is prepared by in-situ polymerization of DOL (1,3-dioxolane) on this framework to achieve safe and stable high-voltage lithium metal battery (LMB). The dual stable electrode interfaces (CEI and SEI) constructed by in-situ can effectively suppress the generation of lithium dendrites and suppress the degradation of the high-voltage NCM811 positive electrode structure and the generation of cracks in NCM811 particles, endowing the battery with extraordinary performance. The as-obtained CSE exhibits high ionic conductivity of 1.01 × 10 −3 S cm −1 at 30 °C, the enlarged electrochemical window of 6.0 V, and the Li + transference number is 0.72. The assembled Li|NCM811 battery is capable of stable cycling for 400 cycles at a cut-off voltage of 4.5 V and current density of 1C, with a capacity decay of only 0.074 % per cycle. .
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Xiaodong Wang,Zijun Liu,Miaomiao Zhou,Ao Li,Ruiping Liu
Elemental interdiffusion and interfacial side reactions between sulfide solid-state electrolytes (SSEs) and nickel-rich layered oxide cathodes inevitably form high-impedance, ion-insulating phases at cathode/electrolyte (C/E) interface, which severely degrades the electrochemical performance of all-solid-state lithium batteries (ASSLBs). Herein, we propose a crystallinity-tailored TiNb 2 O 7 (TNO) coating strategy for LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathodes and the long-term interfacial stability of NCM811/SSE interfaces. The ion-conductive yet electron-insulating TNO coating not only guarantees rapid Li + migration across the C/E interface but also effectively suppresses the oxidative decomposition of SSEs at high voltage. More importantly, compared with the high-crystallinity TNO coating, the low-crystallinity counterpart exhibits superior structural adaptability, which can well accommodate the volume changes of NCM811 during Li + insertion/extraction. This unique structural advantage endows the TNO coating with durable protective capability for NCM811 cathodes, especially under high-current-density cycling conditions. Benefiting from the above synergistic effects, the NCM811 cathode modified with low-crystallinity TNO coating synthesized at 500°C (NCM811@T500) delivers a high specific discharge capacity of 150.9 mAh g − 1 after 100 cycles at 0.069 mA cm − 2 and 25°C. This work provides a novel crystallinity-regulation strategy for cathode surface modification, and offers valuable insights into the rational design of high-performance protective coatings for nickel-rich cathodes in sulfide-based ASSLBs.
✓ 已验证
DOI
高影响因子
Frontiers in Energy Research
·
2022
·
IF 3.858
Zhang Yongquan,Zhu Baoshan,Chi Qingguo,Gao Hongchang,Zhang Changhai,Zhang Tiandong,Zhu Kai,Cao Dianxue
The transport performance of lithium ions affects the rate performance of the cathode at different current densities. The poor interface contact between a solid electrolyte and the cathode makes it difficult to transport lithium ions. Adding a solid electrolyte into the cathode material can improve lithium ion transport. In this paper, we prepared some cathodes with different doping ratios, including two common cathode materials (LiFePO4 and NCM811), and tested their rate and long cycle performance. LFP-10 has a specific discharge capacity of 79.75 mAh g−1 at 5C, and the Li+ diffusion coefficient of LFP-10 is 4.91 × 10−13 cm−2 s−1, which is about 13.4 times higher than the pure LiFePO4 sample. The rate performance of an all-solid-state battery has also been improved, and there is still more than 100 mAh g−1 capacity reserved at 60°C and 2C current density. This shows that the introduction of a PEGDA-based solid electrolyte can significantly improve the Li+ transport of the cathode, and the composite cathode also provides support for the future application of all-solid-state batteries.
研究领域:
材料科学
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电化学
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电池技术
✓ 已验证
DOI
高影响因子
IONICS
·
2025
·
IF 2.6
Wang Yuhang,Ren Zhiqi,Sun Jiaxiu,Li Xinze,Huang Bin,Yang Jianwen
In this work, the effect of potassium permanganate (KMnO 4 ) pre-oxidation treatment on the electrochemical properties of LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) cathode materials was investigated. X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) tests revealed that the pre-oxidation treatment promoted the oxidation of Ni 2+ to Ni 3+ and the formation of a stable Mn-rich surface. Electrochemical testing showed that the electrochemical performance of the NCM811 material pre-oxidized with an appropriate amount of KMnO 4 (811–3) was significantly improved at both ambient (25 ℃) and elevated temperatures (55 ℃) compared to the untreated sample. Additionally, the air stability of 811–3 was enhanced. Specifically, the pre-oxidation treatment increased the oxidation state of nickel, minimized side reactions with CO 2 and moisture in the air, and improved cycling stability, rate performance, and lithium-ion diffusion. It also resulted in a lower self-discharge rate, ensuring better long-term voltage retention. These results indicated that KMnO 4 pre-oxidation is an effective strategy for improving the electrochemical performance of NCM811 and has the potential for application to other Ni-rich cathode materials.
研究领域:
材料科学
·
电化学
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表面工程
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储能技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yali Wang,Nanxi Dong,Bingxue Liu,Kexin Qi,Guofeng Tian,Shengli Qi,Dezhen Wu
The Ni-rich layered oxide cathode (LiNi 0.8 Co 0.1 Mn 0.1 O 2 , NCM811) suffers from serious interfacial side reactions and phase transition during high-voltage cycling (4.7 V), causing the poor rate capability and sharp capacity fading. Herein, a beneficial strategy is proposed, combining rigid/flexible chains, to exploit an endurable poly(imide-siloxane) (PIS) binder with transitable ion channel by structural tailoring and copolymerization. The in-situ formed nanoscale PIS layer on the NCM811 particle surface provides stern resistance to extreme conditions and strong attractive interactions, which enable a firm cathode-electrolyte interface and facile ion transfer path during charge-discharge process. The fabricated PIS-based cathodes under 4.3 V cutoff voltage exhibit higher capacity retention (83% vs. 69%, 1.0C, 500 cycles) and higher rate capacity (137.6 mAh g −1 vs. 123.6 mAh g −1 , 5.0C), in contrast to the cathodes with polyvinylidene fluoride (PVDF) binder. Further test under 4.7 V cutoff voltage indicates the rate capacity of PIS-based cathodes is superior than that of PVDF-based cathodes (163.2 mAh g −1 vs. 119.7 mAh g −1 , 5.0C), as well as superior capacity retention (74 % vs. 34%, 0.2C, 100 cycles). This work provides a valuable guideline for designing a polymer binder by focusing on stabilizing high-voltage cathode structure and facilitating ion diffusion.
研究领域:
材料科学
·
电化学
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电池技术
✓ 已验证
DOI
高影响因子
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
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电化学
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能源存储
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固态离子学
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电池技术
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高分子化学
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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
·
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
·
材料科学
·
能源存储
·
锂离子电池
·
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
·
储能技术
·
材料科学
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电池技术
·
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
·
电极材料
·
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
危险品化学品经营许可证（带存储）