ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yijing Qiu,Dongsheng Lu,Yunyan Gai,Yuepeng Cai
Adiponitrile (ADN) is studied as an additive of commercial carbonate electrolyte for a graphite/NCM811 Li-ion cell in this work. Compared with the cell using a baseline electrolyte, the cycling stability of the cells using 0.2, 0.5, 1, and 2 wt % ADN-added electrolytes is significantly improved. Among them, the effect is most prominent when the ADN content is 0.5 wt %, and the capacity retention rate of the cell after 200 cycles at 0.3 C is increased by 17.6%. Scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy analyses confirm that ADN can make the coating layer formed on the cathode and anode surfaces of the cell denser and uniform. The formation of the cathodic coating layer does not obey the usual mechanism of adsorption between the nitrile group and metal ions, but it may be due to the polymerization of ADN initiated by carbocations from the oxidation of solvent molecules (ethylene carbonate/ethyl methyl carbonate) in the electrolyte. The cathodic coating layer greatly decreases the oxidation of the electrolyte so that a stable coating layer (also called solid electrolyte interface/SEI) can be formed on the anode, which is the reason for improvement of the cycling performance of the cell. However, the formation of the anode SEI layer is almost independent of ADN, and it still depends on the common reduction reaction of the electrolyte.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Kai Huang,Xulin Mu,Yang Ding,Jinhui Li,Manling Sui,Pengfei Yan
Polycrystalline Ni-rich layered lithium transition metal oxides are one of the most promising cathode materials for next-generation high energy density lithium-ion batteries, yet they are still facing many challenges, especially for the cycling induced structural degradations. Intergranular cracking has been identified as one of the most crucial degradations, and grain boundary (GB) engineering has been demonstrated to be an effective countering strategy. Herein, we report a GB modification protocol that can realize not only improved GB stability but also interfacial reaction kinetics, realizing much improved cycling performance of NCM811. The simple and effective solution method can incorporate Ti-dopant into GBs and secondary particle surface, realizing the increase of the capacity retention from 79.5% to 93.5% at 3.0–4.5 V after 100 cycles, and its high voltage (4.7 V) and high temperature (55 °C) cycling stability are also significantly improved. Comprehensive microstructure and electrochemical characterizations of the samples before and after cycling are conducted to reveal the underlying mechanisms, validating that both interfacial degradations and bulk failures have been effectively mitigated. This work provides an effective protocol in the modification of GBs and interfaces of polycrystalline battery materials, which is promising and feasible for industrial mass-production application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Xinru Tan,Maolin Zhang,Dongyan Zhang,Yangxi Yan,Yuan Wang,Zhimin Li
The formation of micro-cracks in Ni-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode particles is an extremely important factor affecting the electrochemical characteristics after long-term cycling. Generally, cracks can be divided into intergranular crack and intracrystalline crack according to their positions. Coating has been confirmed as a highly effective strategy to relieve intergranular cracks. However, the intracrystalline cracks of primary-like particles have rarely been studied. In this work, ethoxy functional polysiloxane (EPS) was directly coated on the surface of original NCM811 by tetraethyl orthosilicate (TEOS) hydrolytic polycondensation method without any additives. Then, the microstructure, micromorphology, surface state and electrochemical properties were investigated in detail by XRD , SEM, TEM, CV and EIS . The results displayed that the micro-cracks of primary-like particles were effectively suppressed under appropriate EPS coating. Accordingly, excellent capacity retention of 95.6% (100 cycles, 1C) and rate performance (144.6 mA h/g, 5C) were obtained. These improved mechanical and electrochemical properties are considered to be related to the EPS stress buffer layer , suppressed oxygen vacancies , inhibited phase transition and reduced volume change.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Omega
·
2021
·
IF 3.512
Mingyu Zhang,Chaoyong Wang,Junkai Zhang,Gang Li,Li Gu
LiNi0.8Co0.1Mn0.1O2 (NCM811) became a research hot point because of its low cost, environmental friendliness, and excellent electrochemical performance. However, Li+/Ni2+ intermixing is an essential factor affecting its applicability. Doping could be an important method to improve the electrochemical performance of NCM811-based cathode materials. In this work, La and Al co-doped NCM811 was prepared by a solid-state method. Results from X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive spectroscopy (EDS) and electrochemical performance were discussed in depth. These showed that when La and Al doping concentrations were 1 and 0.5%, the samples showed the best performance. The as-improved performances were mainly attributed to the reduced Li+/Ni2+ intermixing, suppressed phase transition, and decreased potential polarization and impedance.
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
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Wen-Qing Wang,Cong Xia,Chen-Ting Zhu,Yue-Yang Wu,Jian-Hua Cao,Yue Li,Da-Yong Wu
Li1+xAlxTi2–x(PO4)3 (LATP) is a NASICON-type solid electrolyte that presents stability in aqueous media and high ion conductivity. With these advantages, it is expected to be used as a cathode and separator coating material for lithium-ion batteries to improve battery performance. However, it also displays a high level of residual moisture introduction due to its strong water absorption. Meanwhile, LATP particle size is a key influential factor for the residual moisture level and thereby produces an impact on the battery performance. In this research, we prepared three different particle sizes of LATP (100, 500, and 1000 nm) to investigate their effects as separator coatings on residual moisture and NCM811 battery performance. The results indicate that the water absorption of LATP is much higher than that of Al2O3 with the same particle size; the use of nanoscale LATP keeps the residual moisture of the LATP/PE separator rather high. When the particle size is in the range of 100–1000 nm, the battery’s cycling performance gradually deteriorates with the decrease of the particle size, among which the degradation of rate performance is more noticeable. More importantly, the research finds that LATP particles coated with polydopamine (PDA) can effectively reduce the coating’s residual moisture. After being coated with PDA, LATP particles with a particle size of 1000 nm result in the residual moisture content within the composite separator decreasing from 2136 to 408 ppm, thereby contributing to the optimal performance of NCM811||Li and NMC811||C batteries.
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
ACS Applied Energy Materials
·
2023
·
IF 6.4
Yujie Wang,Chengyun Wang,Huangwang Mai,Weizhen Fan,Haosen Fan,Wei Yang,Fengming Ren,Shengzhou Chen
Although LiNi0.8Co0.1Mn0.1O2 (NCM811) has been widely used in lithium-ion batteries (LIBs) as cathode materials, the high content of nickel typically leads to performance deterioration and other safety issues due to the catalytic decomposition of electrolyte. Herein, we propose a strategy to improve the stability of electrolyte by adopting anhydride-based additives with benzene group (e.g., 6FDA, FPA, and PSA). The theoretical calculation, electrochemical test, and structural characterization indicate that the addition of PSA enables NCM811 to better cycling performance at high, ambient, and low temperatures for pouch cells with SiO/graphite as the anode owing to its higher reduction potential in comparison with that of 6FDA and FPA.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Batteries & Supercaps
·
2024
·
IF 5.1
Jian-Hua Cao,Peng Zhang,Ya-kun Wang,Da-Yong Wu
Graphical 2,2,2-trifluoroethyl phosphite (DETFPi), 1,3-Dioxolane (DOL) and trimethylolpropane tri(methacrylate) (TTE) were polymerized under LiBF 4 initiator on the LATP/PE/LATP separator and thereby obtained DETFPi-PDOL/LATP composite electrolyte after 24 h at room temperature. LATP coating on the surface of the PE separator can improve the cycling stability, rate performance, and interface state of NCM811 batteries. 1,3-Dioxolane (DOL) can undergo in-situ polymerization in batteries to form solid-state organic electrolyte PDOL. When applied to NCM811||Li battery system, PDOL electrolyte helps optimize the contact and interface stability between electrolyte and electrodes. This study explores the effects of PDOL with PE separators coated with Li1 .3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) on the performance of NCM811||Li batteries. 2,2,2-trifluoroethyl phosphite (DETFPi), was mixed with DOL at a 1 : 35 mass ratio. Then, LiBF 4 was used to initiate in-situ polymerization and thereby obtained DETFPi-PDOL electrolyte after 24 h at room temperature. The composite electrolyte exhibits enhanced ion conductivity (1.59×10 −4 S cm −1 ), high lithium ion transference number (0.78), wide electrochemical stability window (4.53 V), and high critical current density (2.2 mA cm −2 ). Li||PDOL@LATP||Li battery shows extremely low overpotential (35 mV) after a constant current stable cycle of 500 h at 1.0 mA cm −2 . After 500 cycles at 1 C, the remaining capacity is 153.9 mAh g −1 with a capacity retention of 82.1 % in NCM811||PDOL@LATP||Li batteries. This indicates that the LATP coating on the surface of the PE separator plays an important role in optimizing the performance of DETFPI-PDOL electrolyte batteries. LATP and DETFPI-PDOL are effective in improving the cycling stability, rate performance, and interface state of NCM811 batteries.
研究领域:
材料科学
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电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Changqi Wang,Yongjun Kang,Bingxue Liu,Daolei Lin,Guofeng Tian,Shengli Qi,Dezhen Wu
Polyimide (PI) is a promising binder material for lithium-ion batteries due to its excellent mechanical strength, high thermal stability, and outstanding chemical inertness. However, the high-temperature imidization requirement (>300 °C) of traditional PI binders is incompatible with current electrode preparation processes, severely limiting their practical applications. In this study, a low-temperature-imidized polyimide (∼150 °C) was elaborately designed and utilized as NCM811 cathode binder, which works by covalently bonding 5-aminobenzimidazole (ABZ) to the ends of the flexible 4,4′-oxidiphthalic anhydride (ODPA)/4,4′-oxidiphenylamine (ODA) poly(amic acid) (PAA) chains to realize the self-catalysis at a low temperature, followed by the assistance of dual-functional N,N′-carbonyldiimidazole (CDI) as a catalyst and dehydrating agent to accelerate the condensation and low-temperature dehydration of amic acid, yielding the imidization of the PAA precursor to give PI at 150 °C. Compared to the conventional PVDF binder, the cathode utilizing this low-temperature imidized polyimide (LTPI) binder exhibited excellent capacity retention (84.9% vs 81.7%) after 100 cycles at 0.2C, and superior rate performance (119.3 mAh·g–1 vs 95.7 mAh·g–1 at 5.0C) under a 4.3 V cutoff voltage. The CV, SEM, XRD, and XPS results demonstrate that the designed LTPI binder effectively suppresses the hexagonal (H2) to hexagonal (H3) phase transition and transition metal dissolution, maintaining the cathode’s structural integrity during charge–discharge cycles, thereby ensuring excellent long-term cycle stability. Furthermore, the NCM811 cathode with LTPI binder exhibits significantly enhanced flame-retardant performance compared with the NCM811/PVDF cathode in the combustion experiments, demonstrating the superiority of LTPI binders in improving the safety of the cathode materials. The NCM811/LTPI cathode retains the excellent structural and electrochemical stability of traditional high-temperature-imidized PI binders, providing a practical pathway to develop high-performance binder materials for high-safety and long-cycling lithium-ion batteries.
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
RARE METALS
·
2024
·Vol. 44
·期 3
·1577-1593
·
IF 9.6
Sun Gao-Xing,Zhu Bin,He Rui,Liang Qi-Dong,Jiang Sheng-Yu,Ren Yan,Pan Xiao-Xiao,Sun Yu-Qing,Lu Mi,Zhang Wen-Xian,Huang Cheng-Huan,Zhuang Shu-Xin
Although lithium-ion batteries are widely recognized as a new generation of energy storage devices, their large-scale application is severely hampered by their low energy density and restricted cyclic stability. Herein, an ingenious dual-modified interface, where the F-doping and fluorocarbon coating co-existed on Li[Ni 0.8 Co 0.1 Mn 0.1 ]O 2 surface, is rationally constructed to elevate its energy density and structural stability attributed to F − grafting between the bulk material and the coating utilizing a robust super-conformal fluorocarbon coating structural framework and more stable F-doped system under high charge/discharge cut-off voltage. In comparison with a single carbon-coated modified Li[Ni 0.8 Co 0.1 Mn 0.1 ]O 2 , the dual-modified sample overcomes the fatal disadvantage of carbon coating stripping during long-period cycles ascribed to the “TM-F-multifunctional coating” connector which firmly combines the bulk material with the coating with a strong interaction force, exhibiting a more stable-reversible structure and excellent comprehensive electrochemical performance under high cut-off voltage. Concomitantly, the F-transition metal bonds with stronger bond energies improve its structural reversibility during the processes of charge/discharge under high voltage. Furthermore, the fluorocarbon coating enhances its charge transfer ability and effectively restrains the interfacial side reactions. Additionally, the climbing nudged elastic band methodology is used to calculate the diffusion energy barrier of lithium-ions in the matrix material, which confirms the fundamental reason for its superior lithium-ion diffusion ability. The high pseudocapacitance contribution ratio is perfectly explained by calculating the adsorption capacity on the surface of the dual-modified sample. Consequently, experiments and theoretical calculations unequivocally confirm its distinguished electrochemical properties under high cut-off voltage. Graphical
研究领域:
材料科学
·
电化学
·
能源存储
·
锂离子电池
·
表面工程
·
固态化学
·
纳米材料
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Lucheng Li,Meiling Liu,Peng Yang,Wenfeng Yuan,Jun Chen
Broadening the charging and discharging voltage window of high nickel cathode material NCM811 is the most expected method to improve the high specific energy density of batteries currently, yet the cathode-electrolyte interface (CEI) formed by the oxidized and decomposed products of carbonate-based electrolyte under high voltage are always so unsatisfied. Therefore, a voltage-stabilizer, TPFPB (Tris(pentafluoro)phenylborane), added into baseline electrolyte (1 M LiPF 6 in EC:EMC:DMC=1:1:1 vol%) to promote the electrochemical performance of the battery at 4.5 V. The results interpret that the TPFPB-contained NCM811-Li half-cells exhibit high specific capacity (167.10 mAh/g), excellent capacity retention rate (CRR) (75.37 %), and high rate performance (173.3 mAh/g at 5C) during 4.5 V. Meanwhile, through the analysis of the physical characterization techniques. the B- and F-rich interfacial layer, named as CEI film, existing at the interface between the cathode and the electrolyte, produced under 4.5 V, is superior, resulting in impeding the structural collapse of the cathode material and the continued dissolution of transition metal ions (TM n + ) from the cathode material, as well as, ameliorate the electrochemical polarization of the battery, ultimately, it can stabilize the electrochemical performance of the battery under high voltage. Therein, the present work elucidate a new and substantial approach to enhance the high-voltage performances of rich-Ni cathode materials.
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
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
ACS Nano
·
2025
·
IF 16
Chong Xu,Shuang Liu,Sai Che,Guang Ma,Gong Cheng,Dongyuan Zhang,Junjie Fu,Ye Wang,Jiahao Yang,Yuci Tian,Yongpeng Cui,Weihua Chen,Yongfeng Li
Incorporating lithium nitrate (LiNO3) as a film-forming additive into carbonate-based electrolytes presents a promising strategy to enhance the stability of high-energy-density Li||NCM811 batteries. However, the small size of Li+ and the high donor number (DN) of NO3– hinder the dissociation of LiNO3, and its limited solubility (<800 ppm) in carbonate-based electrolytes poses significant challenges for practical application. To address this issue, we propose a “Small-Sized Carrier” strategy that enhances the solubility of LiNO3 in carbonate solvents by modulating the intermolecular interactions within the solvent system. This approach employs vinylene carbonate (VC), a small molecule with moderate polarity, to enhance the dissolution of LiNO3 without compromising the compatibility of the electrolyte with the lithium metal anode. The introduction of the “Small-Sized Carrier” additive system simultaneously enhances the stability of the electrode–electrolyte interfaces and optimizes the solvation structure of the electrolyte. As a result, the electrolyte developed through this strategy demonstrates outstanding electrochemical performance, with Li||NCM811 batteries achieving a capacity retention of 83.8% after 600 cycles. This work provides an insightful approach to designing advanced electrolytes tailored to high-energy-density lithium metal batteries (LMBs).
研究领域:
电化学
·
储能材料
·
电池技术
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）