CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wei-Chen Zheng,Jin-Xia Lin,Hui Chen,Shi-Shi Liu,Chen-Guang Shi,Ling Huang,Shi-Gang Sun
Ni-rich layered oxides are considered ideal positive electrode materials for next-generation state-of-the-art Li-based batteries owing to their high energy densities. However, the structural degradation of Ni-rich positive electrodes and electrolyte decomposition presents significant challenges, particularly at high cut-off voltages. Herein, we report a novel electrolyte consisting of fluorinated solvents that enables the long lifespan of a Li||LiNiO 2 cell with a cut-off voltage of up to 4.5 V. The Li||LiNiO 2 cell retains 93.8% of its initial capacity after 200 cycles. The cycling stability was ascribed to the fluorinated solvents dominating the first structural shell of Li + and deriving a robust cathode-electrolyte interphase (CEI) on the positive electrode. Compared to commercial electrolytes, the fluorinated electrolyte inhibits the structural degradation, stress corrosion cracking, and interphase side reactions of the LiNiO 2 electrode. On the Li negative electrode side, ideal Li plating/stripping and the inhibition of the attack of Ni 2+ are achieved. Furthermore, the 4.5 V-Li||LiNiO 2 cell exhibited a capacity retention of 80.2% after 100 cycles, even under extremely fast-charging conditions.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Ziye Wang,Qianchen Wang,Yingshuai Wang,Tinglu Song,Yuhang Xin,Qingbo Zhou,Lei Liu,Amna Safdar,Feng Wu,Hongcai Gao
Lithium metal batteries (LMBs) are regarded as the next generation of electrochemical energy storage devices with high energy density that hold great promise in the applications of electric vehicles (EVs) and portable electronic devices. However, the commercial carbonate electrolytes are limited by their flammability, lithium dendrite growth and poor cycle stability. In this work, an ultra-low concentration and flame-retardant electrolyte with 0.2 M lithium hexafluorophosphorate (LiPF 6 ) solventated in fluoroethylene carbonate (FEC), dimethyl carbonate (DMC) and 1,1,2,2-tetrafluoroethylene-2,2,3,3-tetrafluoropropyl ether (TTE) was prepared for lithium metal batteries. The results demonstrate that the introduction of a large amount of fluorine-containing solvent formed a uniform, strong and thin electrolyte/electrode interface layer both on the cathode and anode. That efficiently suppressed dendrite formation on the lithium metal anode, and greatly reduced the appearance of undesirable decomposition products, ensuring the cycling stability of electrolyte and electrode materials. Notably, the ultra-low concentration electrolyte has excellent flame retardancy, and significantly improves the electrochemical characteristics of Li||Li symmetrical batteries and Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) batteries. The work presents a promising non-flammable, low-concentration electrolyte for next-generation LMBs and new insights into innovations in the formulation of advanced electrolytes for electrochemical energy storage technologies.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
CHINESE CHEMICAL LETTERS
·
2025
·
IF 8.9
Bin Wang,Qingqing Zhou,Junjie Lu,Chuyang Li,Mengmeng Fan,Wenwei Ding,Bifu Sheng,Wenjuan Zhu,Qian Ni,Huixin Chen,Xiang Han
Poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP)-based solid polymer electrolytes show great potential for high energy lithium metal batteries, however, the residual solvent and related severe side reactions limit its development. Herein, a PVDF-HFP-based solid polymer electrolyte modified by fluorobenzene (FB) co-solvent is designed to address these problems. The introduced FB with weak solvation interaction regulates the coordination environment and induces anions to enter the solvation structure, generating more contact ion pairs (CIPs) and aggregates (AGGs). In addition, the anions-derived LiF-rich interphases help to improve the interface stability against Li metal. As a result, the FB-PVDF-HFP achieves high ionic conductivity (4.1 × 10 −4 S/cm) and low activation energy (0.125 eV) at room temperature. In addition, Li||Li symmetric cells using FB-PVDF-HFP electrolyte can achieve uniform and dendrite-free lithium deposition/stripping in the long-term cycling over 2300 h. The assembled solid-state Li|FB-PVDF-HFP|LFP full cell shows improved rate performance and cycling performance (600 cycles at 0.5 C and 450 cycles at 3 C) at room temperature. This work verifies the feasibility of fluorinated terminated solid polymer electrolytes on its lithium-ion transport and interfacial stability in lithium metal batteries.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Siru He,Jianwei Xiong,Huimin Yuan,Peide Zhu,Wenbo Peng,Xingzhu Wang,Baomin Xu
Continuous side reactions between conventional carbonate-based electrolytes and electrodes lead to electrolyte consumption and the growth of lithium dendrites, which always lead to serious capacity fading or safety issues, hindering the development of lithium metal batteries. Here, a nonflammable all-fluorinated electrolyte with the anion-participating Li+ solvation sheath is developed and the corresponding electrochemical properties are studied. Combining theoretical calculations and X-ray photoelectron spectroscopy analysis, ethyl 2,2,2-trifluoroethyl carbonate (ETFEC) and methyl difluoroacetate (MDFA) as cosolvents in the all-fluorinated electrolyte, PF6– anions accumulate on the lithium metal anode and preferentially reduced to obtain a LiF-rich solid electrolyte layer, inducing uniform lithium metal deposition. Additionally, the anions located in the solvation structure improve the reduction stability of the solvent, which avoids the rapid decline in battery capacity caused by the continued decomposition of the solvent. Consequently, The Li||NCM811 battery achieved initial capacity retention of 71.48% after 430 cycles at a voltage of 4.3 V, and the capacity retention reached 64.52% after 225 cycles even at a high voltage of 4.5 V. This nonflammable electrolyte can alleviate the rapid decline in battery capacity caused by solvent decomposition.
研究领域:
电化学
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能源材料
·
电池技术
·
界面化学
·
材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qingqing Zhou,Chuyang Li,Bin Wang,Wenwei Ding,Junjie Lu,Bifu Sheng,Wei Li,Wenjuan Zhu,Qian Ni,Xiang Han
Polyethylene oxide (PEO)-based solid-state batteries have attracted extensive attention due to their scalable processing, flexible and soft interface contact, and excellent compatibility with lithium metal. The low ionic conductivity at room temperature, caused by the strong interaction between PEO chains and lithium ions , however, limits its practical application. Herein, taking the PEO-PAN dual-matrix polymer electrolyte as an example, a weak coordinated solvation structure is enabled by fluoroethylene carbonate (FEC) as a co-solvent during electrolyte preparation. The tiny residual FEC is demonstrated to weaken the interaction between lithium ions and PEO chains while competitively dissociating lithium salts with the residual solvent and anions. In addition, the incorporation of FEC enhances the dispersion of LATP nanoparticle fillers, which reduces the crystallinity of PEO. Furthermore, the anion-derived LiF-rich solid-electrolyte interphase significantly suppresses the formation of lithium dendrites. Consequently, the prepared PEO-PAN-LATP-LiTFSI-5 % FEC (PPLLF) composite solid polymer exhibits an ambient ionic conductivity of ∼ 1 × 10 −4 S cm −1 and enables stable cycling for over 450 h in a Li||Li symmetrical battery at room temperature. The assembled Li|PPLLF|LFP full battery delivers a specific capacity of 137.6 mAh/g after 300 cycles at 0.2C, further demonstrating the effectiveness of the solvation manipulation strategy.
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DOI
PubMed
高影响因子
Advanced Science
·
2025
·Vol. 12
·期 37
·e17305
·
IF 14.1
Zhicheng Wang,Shixiao Weng,Haiyang Zhang,Liping Wang,Xu Yao,Haifeng Tu,Dan Huang,Suwan Lu,Lingwang Liu,Jiangyan Xue,Fengrui Zhang,Guan Wu,Jieyun Zheng,Qing Wang,Liquan Chen,Jingjing Xu,Hong Li,Xiaodong Wu
The performance of lithium-sulfur (Li-S) batteries is crucially affected by the anodic stability of Li-metal and cathodic conversion kinetics of sulfur-carbon (S/C) composites. Herein, a weakly solvating electrolyte (WSE) with moderate lithium polysulfides (LiPSs) solubility, consisting of 1 M lithium bis(trifluoromethane sulfonyl) imide (LiTFSI) in non-fluorinated solvent of cyclopentyl methyl ether (CPME) and 1,3-dioxolane (DOL) additive, is employed in Li-S batteries to simultaneously achieve high anodic stability and appropriate cathodic kinetics. This WSE exhibits a good capability of suppressing LiPSs shuttling by forming an anions-dominated Li + solvation structure, effectively inducing a stable solid electrolyte interphase (SEI) to guarantee anodic stability of the Li-metal anode. Additionally, the DOL additive in the WSE aids in forming a thin organic-inorganic hybrid cathode electrolyte interphase (CEI) on the surface of S/Li 2 S particles, which maintains good conversion kinetics and suppresses dead S/Li 2 S growth in the S/C cathode. Consequently, Li-S batteries with the WSE deliver a high initial capacity (≈1208 mAh g −1 ), a high average Coulombic efficiency (≈98.6%), and a high capacity retention rate (≈82.4%) over 200 cycles. Stable cycling performance over 100 cycles is also observed in the Li-S pouch cell with the WSE even under harsh conditions.
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PubMed
高影响因子
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