Energy Advances
·
2023
·Vol. 2
·期 10
·1685-1692
·
IF 0
Guozhe Ma,Yu Zheng,Fanbo Meng,Renzong Hu
High-entropy oxides (HEOs) have started to attract widespread interest as anode materials for lithium-ion batteries (LIBs), because of their high theoretical discharge capacities, fast ionic conductivity, and stable structure caused by the unique entropy stabilization effect and the “cocktail” effect. However, the lithiation mechanism of HEO anode is still conversional, which prevents its further development. Herein, we propose an Li2O-doping strategy for improving the lithium storage ability of HEO anodes. Li2O is successfully introduced into the spinel high-entropy oxide to obtain a (FeMgNiCrMnLi)3O4 anode (Li-SHEO) via a solution combustion synthesis and ball milling method. Experimental results show Li doping would induce the growth of oxygen vacancies and regulate the conversion reactions during the discharge process, leading to improved electrochemical performance. As a result, the lithiation process of an Li-SHEO anode includes an enhanced Li+ ion intercalation process and a typical conversion reaction. Compared with the (FeMgNiCrMnLi)3O4 (SHEO) anode, the Li-SHEO anode shows a high reversible discharge capacity of 850.7 mA h g−1 after 200 cycles under a large current density of 2.0 A g−1.
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DOI
Nanomaterials
·
2021
·Vol. 11
·期 10
·2562
·
IF 5.076
Shuang Lian,Yu Wang,Haifeng Ji,Xiaojie Zhang,Jingjing Shi,Yi Feng,Xiongwei Qu
The development of solid-state polymer electrolytes is an effective way to overcome the notorious shuttle effect of polysulfides in traditional liquid lithium sulfur batteries. In this paper, cationic cyclopropenium based cross-linked polymer was firstly prepared with the one pot method, and then the counter ion was replaced by TFSI−anion using simple ion replacement. Cationic cyclopropenium hyper-crosslinked polymer (HP) was introduced into a polyethylene oxide (PEO) matrix with the solution casting method to prepare a composite polymer electrolyte membrane. By adding HP@TFSI to the PEO-based electrolyte, the mechanical and electrochemical properties of the solid-state lithium-sulfur batteries were significantly improved. The PEO-20%HP@TFSI electrolyte shows the highest Li+ionic conductivity at 60 °C (4.0 × 10−4S·cm−1) and the highest mechanical strength. In the PEO matrix, uniform distribution of HP@TFSI inhibits crystallization and weakens the interaction between each PEO chain. Compared with pure PEO/LiTFSI electrolyte, the PEO-20%HP@TFSI electrolyte shows lower interface resistance and higher interface stability with lithium anode. The lithium sulfur battery based on the PEO-20%HP@TFSI electrolyte shows excellent electrochemical performance, high Coulombic efficiency and high cycle stability. After 500 cycles, the capacity of the lithium-sulfur battery based on PEO-20%HP@TFSI electrolytes keeps approximately 410 mAh·g−1at 1 C, the Coulomb efficiency is close to 100%, and the cycle capacity decay rate is 0.082%.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Minjing Chen,Wenyang Wang,Zhepu Shi,Zhaoping Liu,Cai Shen
Solid electrolyte interphase (SEI) grown on electrode surfaces during charge-discharge processes plays a key role in the cycle performance of lithium-ion batteries. In-situ study of cathode electrolyte interphase (CEI) is challenging due to the complicated interfacial reactions on the cathode materials including gas formation and the formation of thin CEI film. Herein, we applied the electrochemical atomic force microscope (EC-AFM) to study the interfacial changes in high energy density Li- and Mn-rich (LMR) materials with an F-rich electrolyte (1 M LiPF 6 FEC/FEMC/HFE). The study indicated that the electrolyte formed a uniform and dense passivation CEI film on the LMR material surface at high voltage. The CEI is composed of inorganic LiF substrate as confirmed by X-ray photoelectron spectroscopy (XPS). The assembled battery (LMR||Li) shows an excellent cycle performance and maintains capacity at 85.5% after 100 cycles, compared to the 13.7% retention rate of commercial carbonate electrolyte (1 M LiPF 6 EC/EMC/DMC).
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DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2022
·
IF 6.364
Kui Liu,Liang Shi,Xueying Wang,Cheng Liu,Jie Li,Yulong Liao,Lichuan Jin,Dainan Zhang,Huaiwu Zhang
Herein, Li + -enriched Li (1+ x )2 ZnTi 3 O 8 ceramics are prepared via the solid-phase methods. As x increases, the unit cell volume gradually increases, while the grain size initially increases and then decreases gradually. The Li (1+0.06)2 ZnTi 3 O 8 ceramics exhibit the best dielectric properties : ε r = 25.92, Q × f = 109534 GHz (@7.37 GHz, which is a 48 % increase compared with the stoichiometric counterpart.), and τ f = −8.21 ppm/°C. The complex chemical bond theory and Raman spectroscopy reveal that Ti-O bonds have a significant effect on the dielectric properties . An optimal Li + enrichment leads to an overall reduction in the distortion of the Li/ZnO 4 tetrahedra, resulting in a reduction in τ f . First-principles calculations demonstrate that a suitable excess of Li + leads to an increase in the band-gap as well as an enhanced electron cloud density in the internal space of the Li1/ZnO 4 tetrahedra, thereby increasing the Q × f . In summary, Li + -enriched Li (1+0.06)2 ZnTi 3 O 8 ceramics are promising for a wide array of applications in microwave communications.
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DOI
高影响因子
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.
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高影响因子
CHEMISTRY OF MATERIALS
·
2015
·
IF 8.354
Xinmiao Liang,Liying Wang,Yangming Jiang,Jian Wang,Huan Luo,Chaoyang Liu,Jiwen Feng
Li10GeP2S12 (LGPS) is a new solid electrolyte of the highest Li ionic conductivity reported as of now. An anisotropic 3D Li ionic transport network consisting of an ultrafast Li 1D diffusion tunnel and fast in-plane 2D pathways was previously predicted by molecular dynamics simulations. In this paper, we have studied in detail the Li ion dynamics in LGPS by multiple solid-state NMR methods. Two different Li motion processes, characterized by apparently different activation energies of 0.16 eV and 0.26 eV, were unambiguously probed by both 7Li and 31P solid-state NMR and assigned to Li ion diffusions in the 1D tunnel and in the 2D plane, respectively. 31P spin-locking relaxation measurement further reveals that interstitial position Li(4) is active for in-plane Li migration.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jingshun Wang,Yongquan Zhang,Zengxu Chen,Shuo Fan,Qihui Zhang,Yue Zhang,Tiandong Zhang,Changhai Zhang,Qingguo Chi
Polymer electrolytes have become widely popular on account of their low expenses, reduced weight, simple processing, and excellent safety features. However, polymer electrolytes have yet to find use in commercial batteries because of their limited mechanical durability and poor ionic conductivity . In this paper, an ultra-stable cycles and interfaces blending polymer electrolyte (BPE) suitable for all solid-state Li metal batteries was prepared by blending three polymers: polymethyl methacrylate (PMMA), polyvinylidene fluoride hexafluoropropylene (PVDF-HFP), and polyethylene oxide (PEO). Microstructure characterization showed numerous amorphous areas with strong interfacial strength of the BPE. The BPE3 exhibited a maximum of 15.65 MPa in tensile strength. BPE2 have excellent electrochemical performance, such as wide electrochemical windows (up to 4.7 V vs Li/Li + ), high lithium ion transference numbers (up to 0.75), high ion conductivity (up to 1.87 × 10 -4 S cm −1 at 60 °C), and excellent interface stability. By assembling all state-solid LiFePO 4 /BPE2/Li batteries for electrochemical testing, BPE2 exhibit high electrochemical characteristics. BPE2 discharge specific capacity is as high as 154.7 mAh g −1 at 1C. The BPE2 underwent 200 cycles at 0.5C and 400 cycles at 1C, with capacity retention rates of 95.7 % and 96.6 %, respectively. BPE is a promising electrolyte candidate for flexible lithium metal batteries.
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DOI
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Zhaoyi Wang,Xiaogang Li,Nanxi Dong,Bingxue Liu,Guofeng Tian,Shengli Qi,Dezhen Wu
Due to the low melting point and non-polarity of polyethylene (PE), the commercially available PE microporous separator intrinsically has poor thermostability above 100 °C and inferior wettability , limiting the development of lithium-ion batteries (LIBs). Herein, a novel PE composite separator coated by high-temperature zirconia@polyimide core–shell nano-microspheres (ZrO 2 @PI nano-microspheres) was designed, producing (ZrO 2 @PI)/PE separator with thermal stability, wettability, and flame retardancy. On account of the ZrO 2 shell nanoencapsulation, the hydrophilicity of PI nano-microspheres has been dramatically improved, which can enhance the electrolyte wettability of the composite separator, and the prepared (ZrO 2 @PI)/PE separator displays enhanced thermal dimensional stability, maintaining its original shape with negligible shrinkage at 150 °C. Furthermore, different from the commercial Al 2 O 3 ceramic-coated separators, the (ZrO 2 @PI)/PE separators possess lower areal density, which is only half as much as the Al 2 O 3 /PE separators. Besides, the half-cell assembled with this (ZrO 2 @PI)/PE separator shows a comparable capacity of 156.9 mAh·g −1 at 5 C to PE separator (118.4 mAh·g −1 ). Meanwhile, the cells assembled with (ZrO 2 @PI)/PE separator demonstrate enhanced cycle performance and thermal safety performance and can work continuously for 109 min at 140 °C, which has enormous improvement compared with the PE-separator-equipped cell (i.e., 21 min). The above results manifest that the (ZrO 2 @PI)/PE separator prepared in this work furnishes LIBs with high safety and electrochemical performance, promising new-generation high energy density and high security LIBs.
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DOI
高影响因子
International Journal of Extreme Manufacturing
·
2022
·Vol. 5
·期 1
·015502
·
IF 10.036
Zhibin Jiang,Lujie Jin,Xiying Jian,Jinxia Huang,Hongshuai Wang,Binhong Wu,Kang Wang,Ling Chen,Youyong Li,Xiang Liu,Weishan Li
Lithium-sulfur (Li-S) batteries can provide far higher energy density than currently commercialized lithium ion batteries, but challenges remain before it they are used in practice. One of the challenges is the shuttle effect that originates from soluble intermediates, like lithium polysulfides. To address this issue, we report a novel laminar composite, N,O-carboxymethyl chitosan-reduced graphene oxide (CC-rGO), which is manufactured via the self-assembly of CC onto GO and subsequent reduction of GO under an extreme condition of 1 Pa and −50 °C. The synthesized laminar CC-rGO composite is mixed with acetylene black (AB) and coated on a commercial polypropylene (PP) membrane, resulting in a separator (CC-rGO/AB/PP) that can not only completely suppress the polysulfides penetration, but also can accelerate the lithium ion transportation, providing a Li-S battery with excellent cyclic stability and rate capability. As confirmed by theoretic simulations, this unique feature of CC-rGO is attributed to its strong repulsive interaction to polysulfide anions and its benefit for fast lithium ion transportation through the paths paved by the heteroatoms in CC.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
FuYin Lan,HaiYan Zhang,Jinchen Fan,Qunjie Xu,Hexing Li,YuLin Min
Herein, we introduce polymer nanofibers of TiO2@NiCo-LDH as interlayers into Li–S batteries. From 0 to 60 °C, the interlayers can deliver high sulfur utilization, an outstanding rate capability, and excellent cycling life. High-temperature excitation makes it easier for the valence band electrons of TiO2 to transition to the conduction band. The electron–hole pairs formed on the surface combine with the ether group of 1,3-dioxolane in the electrolyte, which greatly reduces the decomposition and volatilization rates of the electrolyte, ensuring Li–S batteries with good cycle performance at high temperatures. The capacity can stabilize at 798.6 mAh g–1 after 100 cycles at 60 °C and 1C, and the battery can provide a capacity higher than 323.2 mAh g–1 at 0 °C. Simultaneously, the lithium metal symmetrical battery with a functional separator can be continuously cycled for 1800 and 750 h without a short circuit at the current densities of 0.65 and 1.63 mA cm–2, respectively.
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DOI
高影响因子
CARBON
·
2024
·
IF 10.5
Longfei Wang,Yunhao Zhao,Jiayang Sun,Yuqing Li,Qunting Qu,Honghe Zheng
Natural graphite (NG) is a strong competitor in the anode market of Li-ion batteries because of its low cost, rich resource, low energy consumption and low carbon dioxide emission during production. The main problems inhibiting its universal application are its high surface area and the attendant unstable solid/electrolyte interphase (SEI), leading to unsatisfactory cycling and rate performance. In this work, a Li + -conductive, thermally and mechanically stable organic polymer layer is successfully constructed on NG surface by virtue of the simultaneous polymerization and crosslinking reactions of chitosan (CS) and acrylic acid (AA). With controllable thickness, the polymer layer denoted as CSAA significantly decreases the specific surface area of NG, works as an inner SEI substrate greatly mitigating the decomposition of electrolyte, and induces the formation of a LiF-rich SEI outer layer. The SEI resistance and activation energy for charge-transfer reactions are considerably reduced. Benefiting from the superior properties of CSAA-derived SEI, the NG@CSAA anodes exhibit a high initial coulombic efficiency of 94.1 %, fast charge/discharge capability and prolonged cycle life at both 25 °C and 45 °C in the LiFePO 4 cathodes-based full cells.
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DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2022
·Vol. 27
·期 1
·171-182
·
IF 2.747
He Jielong,Bai Zhe,Huang Xinping,Zhang Zhengyu,Lu Lu,Li Jun
In this work, Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 was prepared by the sol–gel method and coated with FePO 4 . The experimental results show that the material surface is uniformly coated with FePO 4 . A small amount of coating will not change the layered structure of the material. Among them, the material with 5% FePO 4 coating has the best performance. The first charge and discharge specific capacity at 0.1 C current density is 324.4 mAh g −1 and 280.4 mAh g −1 , respectively. And the first coulomb efficiency is 86.4%, which is significantly higher than 75.6% of the pristine material. The improvement of the first charge–discharge performance of the coating material is due to the decrease of discharge voltage plateau and the redox of FePO 4 with electrochemical activity. When the FePO 4 coating content is 5%, the cycling performance of the material at 0.2 C current density is the best. After 100 cycles, the capacity decays from 268.4 to 232.9 mAh g −1 , and the capacity retention rate is 86.78%, which is higher than 60.58% of the pristine sample. The discharge specific capacity of 5% coated material at 5 C rate is 134.8 mAh g −1 , which is higher than 95.3 mAh g −1 of the pristine material. Graphical
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高影响因子
危险品化学品经营许可证（带存储）