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ADVANCED MATERIALS · 2024 · IF 27.4

Unveiling the In Situ Evolution of Li2O-Rich Solid Electrolyte Interface on CoOx Embedded Carbon Fibers as Li Anode Host

Zhimin Hao,Dapeng Liu,Xintao Zuo,Haohan Yu,Yu Zhang

Modification of three-dimensional (3D) carbon hosts with metal oxides has been considered as advantageous for the formation of Li 2 O-rich solid electrolyte interface (SEI), which can show fast Li + diffusion, and meanwhile alleviate dendrite problems caused by fragility and nonuniformity of native SEIs. However, the lack of convincing experimental evidence has made it difficult to unveil the true origin of oxygen in Li 2 O-rich SEIs until now. Herein, CoO x embedded carbon nanofibers (CNF-CoO x ) are successfully prepared as high-performance Li anode hosts. By employing 18 O isotope labeling, the role of CoO x during SEI evolution is elucidated, revealing that CoO x contributes significantly to Li 2 O formation by delivering oxygen. Benefiting from the rich Li 2 O content, the as-formed SEIs greatly improve the Li + migration kinetics, and therefore, the CNF-CoO x @Li anode can exhibit excellent cycling stability in half, symmetrical, and full cells.

研究领域: 材料科学 · 电化学 · 电池技术
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Chemistry-An Asian Journal · 2022 ·Vol. 17 ·期 22 ·e202200839 · IF 4.839

Poly(ethylene oxide)-Based Composite Electrolyte with Lithium-Doped High-Entropy Oxide Ceramic Enabled Robust Solid-State Lithium-Metal Batteries

Weijie Liu,Jianbo Jiang,Zhihao Yang,Yang Liu,Zhengfei Yang,Manman Bu,Shuangxiong Liao,Weiying Wu,Tieqi Huang,Shangbin Sang,Hongtao Liu

Solid polymer electrolytes using poly(ethylene oxide) (PEO) as matrix are mostly applied due to the superior Li + transfer ability of oxyethyl chain. However, the high crystallinity, low oxidation potential window, and insufficient mechanical strength hinder PEO deployment in solid-state batteries. Here, a novel composite solid electrolyte combined PEO with a lithium-doped high-entropy oxide (Li 0.25 HEO) ceramic powder is presented, which exhibits excellent properties for solid-state lithium metal battery applications. On one hand, the rich oxygen vacancies of Li 0.25 HEO surface are favorable to capturing anionic groups (e. g. TFSI − ), reinforcing the Li + dissociation. On the other hand, Li 0.25 HEO with abundant Lewis acid sites markedly promotes the PEO oxidation potential window. Additionally, the incorporation of Li 0.25 HEO ceramic powder can effectively inhibit the PEO crystallization and enhance the mechanic strength of the composite electrolyte as well. The assembled solid-state lithium metal battery based on the composite solid electrolyte exhibits high rate capacity and durable cycle performance, showing potential development and application prospects.

研究领域: 材料科学 · 电化学 · 电池技术
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MOLECULES · 2022 ·Vol. 27 ·期 21 ·7488 · IF 4.927

Novel In Situ Growth of ZIF-8 in Porous Epoxy Matrix for Mechanically Robust Composite Electrolyte of High-Performance, Long-Life Lithium Metal Batteries

Wenjie Zhang,Jianlin Long,Haijun Wang,Jinle Lan,Yunhua Yu,Xiaoping Yang

Polymer electrolytes (PEs) with high flexibility, low cost, and excellent interface compatibility have been considered as an ideal substitute for traditional liquid electrolytes for high safety lithium metal batteries (LMBs). Nevertheless, the mechanical strength of PEs is generally poor to prevent the growth of lithium dendrites during the charge/discharge process, which seriously restricts their wide practical applications. Herein, a mechanical robust ZIF-8/epoxy composite electrolyte with unique pore structure was prepared, which effectively inhibited the growth of lithium dendrites. Meanwhile, the in situ growth of ZIF-8 in porous epoxy matrix can promote the uniform flux and fast transport of lithium ions. Ultimately, the optimal electrolyte shows high ionic conductivity (2.2 × 10−3S cm−1), wide electrochemical window (5 V), and a large Li+transference number (0.70) at room temperature. The Li||NCM811 cell using the optimal electrolyte exhibits high capacity and excellent cycling performance (83.2% capacity retention with 172.1 mA h g−1capacity retained after 200 cycles at 0.2 C). These results indicate that the ZIF-8/epoxy composite electrolyte is of great promise for the application in LMBs.

研究领域: 材料科学 · 电化学 · 能源存储
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ENERGY & FUELS · 2024 · IF 5.2

Enhanced Ionic Conductivity toward Air-Stable Li4SnS4 Solid Electrolytes Achieved by Soft Acid Bi3+ Doping

Lihao Zheng,Juntao Shi,Gaoya Ren,Tiantian Tang,Yefeng Yang,Shenghui Shen,Zhujun Yao

Sulfide solid electrolytes have emerged as highly promising candidates for an all-solid-state battery, while phosphorus-free compounds with air stability have not gotten enough attention. In this study, we focus on an air-stable compound, Li4SnS4, whose structure can be adjusted by Bi3+ doping through the combination of a two-step ball milling method and thermal annealing. The successful substitution of Sn4+ by Bi3+ with lower valence and larger ionic radius results in the enhancement of Li+ concentration in electrolytes and lattice volume, benefiting the Li+ migration. Therefore, the modified glass-ceramic Li4.025Sn0.975Bi0.025S4 exhibits an ionic conductivity of 1.35 × 10–4 S cm–1 at room temperature, which is twice as high as that of pure Li4SnS4. Moreover, the soft acid characteristic of Bi3+ can further ensure the air stability of Li4SnS4 based on the hard and soft acid and base theory. The findings revealed from this research provide a potential avenue for improving the performance of air-stable Li4SnS4 solid-state electrolytes for future large-scale applications.

研究领域: 材料科学 · 电化学 · 能源存储
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Polymers · 2024 ·Vol. 16 ·期 21 ·2972 · IF 4.7

Bilayer Heterostructure Electrolytes Were Prepared by a UV-Curing Process for High Temperature Lithium-Ion Batteries

Qiankun Hun,Lingxiao Lan,Xuanan Lu,Qicheng Hu,Xinghua Liang,Yifeng Guo,Yujiang Wang

Solid-state electrolytes are widely anticipated to revitalize high-energy-density and high-safety lithium-ion batteries. However, low ionic conductivity and high interfacial resistance at room temperature pose challenges for their practical application. In this work, the dual-matrix concept is applied to the design of a bilayer heterogeneous structure. The electrolyte in contact with the cathode blends PVDF-HFP and oxidation-resistant PAN. In contrast, the electrolyte in contact with the anode blends PVDF-HFP and reduction-resistant PEO. A UV-curing process was used to fabricate the bilayer heterostructure electrolyte. The heterostructure electrolyte exhibits an ionic conductivity of 4.27 × 10−4S/cm and a Li+transference number of 0.68 at room temperature. Additionally, when assembled into LiFePO4/CPEs/Li batteries, it shows a high initial discharge capacity at room temperature (168 mAh g−1at 0.1 C and 60 mAh g−1at 2 C), with a capacity retention of 93.3% after 100 cycles at a current density of 0.2 C. Notably, at 60 °C, the battery maintains a discharge capacity of 90 mAh g−1at 2 C, with a capacity retention of 97.4% after 100 cycles at 0.2 C. Therefore, solid-state batteries using this bilayer heterogeneous structure electrolyte demonstrate promising performance, including effective capacity output and cycling stability.

CAS / MDL: 7791-03-9
研究领域: 材料科学 · 电化学 · 能源存储
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Nano-Micro Letters · 2022 ·Vol. 14 ·期 1 ·1-14 · IF 23.655

Quasi-Solid-State Ion-Conducting Arrays Composite Electrolytes with Fast Ion Transport Vertical-Aligned Interfaces for All-Weather Practical Lithium-Metal Batteries

Li Xinyang,Wang Yong,Xi Kai,Yu Wei,Feng Jie,Gao Guoxin,Wu Hu,Jiang Qiu,Abdelkader Amr,Hua Weibo,Zhong Guiming,Ding Shujiang

The composite gel electrolyte with low tortuosity ion-conducting arrays (GPE/ICAs) exhibiting high room-temperature ionic conductivity (1.08 mS cm −1 ) was successfully prepared by directionally growing ice crystals and in-situ polymerization. The stable and rapid Li + migration through ICAs in the GPE is proved by 6 Li solid-state nuclear magnetic resonance and synchrotron radiation X-ray diffraction combined with computer simulations. Li/LiFePO 4 full cells using GPE/ICAs exhibit excellent cycle performance and high-capacity retention at wide temperature (0–60 °C), which has the potential towards all-weather practical solid-state batteries.

研究领域: 材料科学 · 电化学 · 电池技术
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA · 2024 · IF 4.7

Improvement of ionic conductivity of solid polymer electrolyte based on Cu−Al bimetallic metal-organic framework fabricated through molecular grafting

Liu-bin SONG,Tian-yuan LONG,Min-zhi XIAO,Min LIU,Ting-ting ZHAO,Yin-jie KUANG,Lin JIANG,Zhong-liang XIAO

A composite solid electrolyte comprising a Cu−Al bimetallic metal-organic framework (CAB), lithium salt (LiTFSI) and polyethylene oxide (PEO) was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes. Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.% CAB (PL-CAB-10%) exhibits high ionic conductivity (8.42×10 −4 S/cm at 60 °C), high Li + transference number (0.46), wide electrochemical window (4.91 V), good thermal stability, and outstanding mechanical properties. Furthermore, PL-CAB-10% exhibits excellent cycle stability in both Li−Li symmetric battery and Li/PL-CAB- 10%/LiFePO 4 asymmetric battery setups. These enhanced performances are primarily attributable to the introduction of the versatile CAB. The abundant metal sites in CAB can react with TFSI − and PEO through Lewis acid–base interactions, promoting LiTFSI dissociation and improving ionic conductivity. Additionally, regular pores in CAB provide uniformly distributed sites for cation plating during cycling.

研究领域: 材料科学 · 电化学 · 电池技术 · 聚合物科学
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

A self-supporting solid electrolyte membrane with fibrous network structure for solid state lithium metal batteries

Shijie Lu,Xiaorong Chu,Chunli Li,Zhikun Zhao,Jianxiong Xiao,Borong Wu,Daobin Mu

High ionic conductivity and good interface compatibility have always been two major bottlenecks for solid-state electrolytes. Herein, a composite electrolyte membrane comprising poly (propylene carbonate), PVDF-HFP and Li 6 · 3 La 3 Zr 1 · 4 Ta 0 · 6 O 12 is successfully prepared via electrospinning. With the assistance of succinonitrile, the synthesized solid-state electrolyte exhibits high ionic conductivity (1.32 × 10 −3  S cm −1 at room temperature), oxidation potential up to 4.5 V vs Li/Li + and high Li + transference number (0.81). This desirable performance is attributed to the combination of PPC with good Li + conduction ability and PVDF-HFP with excellent mechanical properties, forming a continuous transport framework within the electrolyte. The introduced active fillers and small molecular additive not only benefit to fast Li + mobility, but also reinforce the stability towards Li metal. Li symmetric cell using the solid-state electrolyte can last for 800 h at a current density of 1.0 mA cm −2 with a low overpotential. The NCM811 cell using the electrolyte membrane shows high initial discharge specific capacity (184.3 mAh g −1 at 1 C) and good capacity retention (80.1% after 300 cycles at 30 °C).

研究领域: 材料科学 · 电化学 · 电池技术 · 纳米技术
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