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IONICS · 2021 ·Vol. 27 ·期 8 ·3339-3346 · IF 2.817

Strippable and flexible solid electrolyte membrane by coupling Li6.4La3Zr1.4Ta0.6O12 and insulating polyvinylidene fluoride for solid state lithium ion battery

Liu Huirong,Li Jianling,Feng Wei,Han Guimei

Commercial lithium-ion batteries have safety risks due to the use of electrolyte-containing flammable organic solvents. The development of all solid-state lithium ion batteries with solid electrolyte is a feasible technical way to improve the safety of batteries. In this work, PVDF-based composite solid-state electrolytes (CSEs) were prepared by coupling Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) and polyvinylidene fluoride (PVDF). The electrochemical performance and interfacial compatibility between composite electrolyte and electrode were improved by the combination of appropriate amount of Li-ion-conducting particles and the insulating polymer. The corresponding solid-state battery of LiFePO 4 |PVDF-LLZTO-CSE| Li is fabricated and delivers initial discharge capacity of 162.4 mAh g -1 , and coulomb efficiency is approximately 98.5%. And the solid-state battery exhibits satisfactory rate capability and cycling stability at room temperature. This study suggests that a combination of the lithium garnet particles and insulating polymer is one of the promising methods to solve the problem of liquid electrolyte.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 电池技术
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MethodsX · 2019 · IF 0

Preparation and in-situ Raman characterization of binder-free u-GF@CFC cathode for rechargeable aluminum-ion battery

Chengyuan Liu,Zhiwei Liu,Hongkun Niu,Cong Wang,Zhaowen Wang,Bingliang Gao,Jingjing Liu,Mark Taylor

We provide a method for preparation of binder-free cathode for rechargeable aluminum-ion batteries (AIBs). Ultrasonicated natural graphite (u-NG) flakes in N-methylpyrrolidone (NMP) is drop-casted to a carbon fiber cloth (CFC) to obtain binder-free u-GF@CFC cathode for AIBs. We also provide an in-situ Raman spectral technology and the corresponding in-situ Raman cell to determine the mechanism of intercalation/deintercalation reactions of the chloroaluminate ions at cathode of AIBs. The in-situ Raman spectra are recorded using a Raman spectrometer combined with a potentiostat/galvanostat model electrochemical workstation. • A simple preparation method of a binder-free u-GF@CFC cathode is suggested. • The u-GF@CFC cathode is obtained by drop-casting ultrasonicated graphite flakes on the surface and internal gaps of the carbon fiber cloth. • The method includes the in-situ Raman spectral technology and the corresponding in-situ Raman cell.

研究领域: 电化学 · 能源材料 · 纳米材料 · 电池技术 · 原位表征
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

V2(PO4)O encapsulated into crumpled nitrogen-doped graphene as a high-performance anode material for sodium-ion batteries

Bin Xiao,Wen-hai Zhang,Peng-bo Wang,Lin-bo Tang,Chang-sheng An,Zhen-jiang He,Hui Tong,Jun-chao Zheng,Bo Wang

Phosphate-based polyanion-structured materials have attracted considerable attention as anode materials in lithium-/sodium-ion batteries due to their stable crystal structure, affordability, and environmental friendliness. V 2 (PO 4 )O was encapsulated into crumpled nitrogen-doped graphene (VPO@N-G) through a facile spray-drying method in which VPO particles were completely encapsulated by N-doped graphene. For the first time, VPO@N-G was explored as an anode material for sodium-ion batteries. The Na + storage behavior of VPO@N-G was systematically investigated at the voltage range of 0.01–3.0 V (versus Na/Na + ). Results indicated that the VPO@N-G anode can deliver a highly reversible discharge capacity of 539 mAh g −1  at 0.05 A g −1 and achieve a highly reversible discharge capacity of 235.9 mAh g −1 even at a high current density of 10 A g −1 . Thus, VPO@N-G can be applied as a high-rate anode material for sodium-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米复合材料 · 无机功能材料
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JOM · 2019 ·Vol. 72 ·期 6 ·2245-2249 · IF 2.305

Low-Cost Fabrication of Silicon Nanowires by Molten Salt Electrolysis and Their Electrochemical Performances as Lithium-Ion Battery Anodes

Zhang Yannan,Zhang Yingjie,Li Xue,Liu Jiaming,Zhang Mingyu,Yang Xi,Huang Mengyang,Xu Mingli,Dong Peng,Zhou Zhongren

The molten salt electrolytic method was introduced to prepare metallic silicon that simply utilizes SiO 2 powder as the raw material and equimolar CaCl 2 -NaCl as the electrolyte under 1.8 V current at 700°C for 5 h. The electrochemically synthesized silicon was in the form of nanowire structures with average sizes of 90 nm in diameter and over 1 μm in length. The current efficiency and specific energy consumption of producing silicon nanowires were calculated to be 79.2% and 8.703 kWh/kg, respectively. Benefiting from the synthesized nanowire structure, the silicon anode exhibited a high initial discharge-specific capacity of 3348.1 mAh/g with an initial coulombic efficiency of 85.2%. The present research provides a straightforward idea to show the feasibility of synthesizing silicon-based material by the molten salt electrolytic method and to introduce the application of synthesized silicon nanowires to lithium-ion battery systems.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 无机合成
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IONICS · 2024 ·Vol. 30 ·期 6 ·3111-3119 · IF 2.4

Study on modification of different amino silanes modified polyacrylic acid for ball milling silicon anode of lithium-ion batteries

Teng Zeyu,Wang Zhilong,Li Zhongcheng,Chen Kanghua

Silicon is a strong competitor for the anode of the next generation of lithium-ion batteries, and ball-milled silicon has broad prospects as a low-cost method for preparing nano silicon. In order to match ball-milled silicon, it is imperative to develop better bonding agents with lower costs. Through adding amino silane coupling agent, the performance of ball-milling silicon anode is enhanced. This study explored the network structure formed by amino silane coupling agent with different chain lengths and polyacrylic acids. Herein, the crosslinked network prepared with 3-[2-(2-aminoethyl amino) ethyl amino] propyl-trimethoxysilane as coupling agent had the best performance, and the initial discharge capacity of the silicon anode prepared by this binder reached 3297.4 mAh·g −1 at a constant current density of 0.5A·g −1 , the initial Coulomb efficiency reached 92.25%. After 100 cycles, the discharge capacity of anode was still maintained at 2229.5 mAh·g −1 with excellent charge/discharge performance.

研究领域: 材料科学 · 电化学 · 纳米材料 · 能源存储 · 高分子化学 · 表面改性
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 31 ·15016-15023 · IF 3.925

From solid waste to a high-performance Li3.25Si anode: towards high initial Coulombic efficiency Li–Si alloy electrodes for Li-ion batteries

Yayue He,Youjia Zhang,Zhenxi Li,Peng-Fei Cao,Huabin Yang,Shilun Gao

As a promising anode material for next-generation high-energy density lithium-ion batteries (LIBs), one of the main technical issues for silicon (Si) electrodes is the low initial Coulombic efficiency (ICE). By a pre-lithiation process, preparation of lithium–silicon (Li–Si) alloy electrodes can efficiently improve the ICE, thus leading to excellent electrochemical performance. Herein, with solid wastes as precursors, we report a cost-efficient approach for the fabrication of Li3.25Si anode materials via simple magnesiothermic reduction and then mechanical alloy reaction methods, combining the advantages of low-cost and high ICE. The prepared Li3.25Si@acetylene black (Li3.25Si@A) electrode exhibits excellent electrochemical performance with a high reversible capacity of 1138.9 mA h g−1 over 90 cycles at a current density of 100 mA g−1 and its ICE is as high as 107.7%, which is superior to that of the commercial Li3.25Si@A electrode. With a simple and low-cost manufacturing process and high ICE, the fabrication process will be definitely meaningful in achieving low-cost and high-capacity anode materials with a prolonged cycle life.

研究领域: 材料科学 · 电化学 · 能源存储 · 可持续材料 · 电池技术
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Nano Energy · 2017 · IF 12.343

TiNb2O7 hollow nanofiber anode with superior electrochemical performance in rechargeable lithium ion batteries

Haoxiang Yu,Hua Lan,Lei Yan,Shangshu Qian,Xing Cheng,Haojie Zhu,Nengbing Long,Miao Shui,Jie Shu

Hollow microstructure always exhibits some special properties in the field of electrochemistry . Here, this study reports the rational design and preparation of TiNb 2 O 7 nanofibers with one dimensional hollow structure via co-electrospinning. The as-electrospun TiNb 2 O 7 hollow nanofibers show high intercalation potential, low charge-charge resistance and fast electrochemical kinetics . The electrochemical results exhibit that the TiNb 2 O 7 hollow nanofibers deliver a reversible capacity of 210.1   mAh   g −1 after 150 cycles at a current rate of 0.4   C, and 158.4   mAh   g −1 after 900 cycles even at a current rate of 10   C with an outstanding capacity retention of 80.6%. The excellent electrochemical performance of nanofibers can be related to the unique morphology of hollow structure. Furthermore, the lithium ions storage mechanism of TiNb 2 O 7 hollow nanofibers is also systematically analyzed, which is related to one two-phase coexistence and two solid-solution processes during the whole charge-discharge cycle. In addition, it is also demonstrated by in situ and ex situ observations that TiNb 2 O 7 hollow nanofibers have outstanding structural stability and electrochemical reversibility. Therefore, the TiNb 2 O 7 hollow nanofibers can be applied as an alternative promising electrode material for the next rechargeable lithium ions batteries .

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 无机功能材料
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CERAMICS INTERNATIONAL · 2024 ·Vol. 50 ·期 22 ·44983-44992 · IF 5.1

Electrochemical properties of tungsten doped LiNi0.9Co0.1O2 lithium-ion battery cathode materials

Shuai Zhao,Hai-lin Ren,Yang Su,Cheng-wei Li,Xiao-min Wang

High-nickel layered cathode materials for lithium-ion batteries have received widespread attention in new energy vehicles for their excellent specific energy and cost advantages, and are considered to be the most promising cathode materials for high-energy density lithium-ion batteries. Despite its many advantages, poor thermal stability and rapid capacity degradation have greatly limited its large-scale application. Ion doping is considered to be an effective way to improve its drawbacks, and in this paper, a series of W-doped LiNi 0.9 Co 0.1 O 2 cathode materials were prepared using WO 3 as a tungsten source. Among them, 1 mol% W doping was the most effective, and its reversible capacity of 204.44 mA g −1 still had 93.25 % capacity retention after 100 this cycles at 1C. Combined with DFT calculations , it is found that the introduction of W does not change the original layered structure and the material transitions from semi-metallic to metallic at lower doping concentrations, resulting in more electrons occupying the Fermi energy levels to enhance its electrical conductivity and leading to an elevated spin state and a lower oxidation state of Ni.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态化学 · 计算材料学
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FUEL · 2023 · IF 7.4

Tailoring triple charge (O2−/H+/e−) conducting nature of Fe-based lanthanum doped samarium oxides for ceramic fuel cells (CFCs)

Muhammad Yousaf,Yuzheng Lu,Majid Niaz Akhtar,Ali Sarosh Khawaja,Khalid Mujasam Batoo,Sajjad Hussain,Asma Noor,Muhammad Akbar,Hu Enyi,M.A.K Yousaf Shah,Naveed Mushtaq,Bin Zhu

Lattice defects in rare earth (RE) doped single-phase semiconductor materials play a key role in structural modifications and physicochemical characteristics, resulting to enhance the ionic conductivity. In this work, we synthesized lanthanum doped samarium oxide with different mole ratios and applied it as a ceramics membrane fuel cell device to enable high peak power density (PPD) at low operational temperatures (520–400 °C). The samples are capable of triple charge H + /O 2− /e − conduction and enhance the catalytic function of the cell in terms of HOR and ORR kinetics by producing lattice defects. The fabricated Sm 1.5 La 1.5 Fe 5 O 12 (2-SLFO) fuel cell device exhibits a high OCV of 1.13 V with a maximum PPD of 864.26 mW/cm 2 at 520 °C. Durability measurement verifies that 2-SLFO-based fuel cell device can be worked for 60 h under fuel cell conditions (H 2 /air) at 520 °C. The first principle calculations using density functional theory (DFT) demonstrate that the higher oxygen vacancy concentration in the 2-SLFO sample may cause to the higher charge-transfer kinetics, subsequent in the enhancement of ions transportation of the fabricated fuel cell device.

研究领域: 材料科学 · 电化学 · 能源材料 · 固态离子学 · 燃料电池技术
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JOURNAL OF POWER SOURCES · 2018 · IF 6.945

Lithiated Nafion as polymer electrolyte for solid-state lithium sulfur batteries using carbon-sulfur composite cathode

Jing Gao,Chunshui Sun,Lei Xu,Jian Chen,Chong Wang,Decai Guo,Hao Chen

Due to flexible property and light weight, the lithiated Nafion membrane swollen with PC (PC-Li-Nafion) has been employed as both solid-state electrolyte and separator to fabricate solid-state Li-S cells. The electrochemical measurements of PC-Li-Nafion membrane show that its Li-ion transference number is 0.928, ionic conductivity of 2.1 × 10 −4  S cm −1 can be achieved at 70 °C and its electrochemical window is 0 ∼ +4.1 V vs. Li + /Li. It is observed that the Li dendrites are suppressed by using PC-Li-Nafion membrane due to its single-ion conducting property. The amounts of Li-Nafion resin binder and conductive carbon in the cathode are optimized as 40% and 10% respectively to make a balance of ionic and electronic conductivities . A thin-layer Li-Nafion resin with a thickness of around 2 μm is fabricated between the cathode and PC-Li-Nafion membrane to improve the interfacial contact and further enhance the specific capacity of the cell. When measured at 70 °C, the Li-S cell delivers a reversible specific capacity of 1072.8 mAh g −1  (S) at 0.05 C and 895 mAh g −1  (S) at 1 C. The capacity retention at 1 C is 89% after 100 cycles. These results suggest that high-performance solid-state Li-S cells can be fabricated with the Li-Nafion polymer electrolyte .

研究领域: 电化学 · 能源材料 · 固态电池 · 聚合物电解质 · 锂离子电池 · 电极界面工程 · 储能技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Ternary stabilization strategies for succinonitrile-based in situ polymerized electrolyte enabling high-performance solid lithium metal batteries

Chenyu Lin,Tianqi Yang,Haiyuan Zhang,Donghuang Wang,Wenkui Zhang,Yao Wang,Yang Xia,Hui Huang,Xinhui Xia,Yongping Gan,Xinping He,Xinyong Tao,Jun Zhang

Solid-state lithium metal batteries with high energy density and safety have gained increasing attention due to their potential applications. However, the practical use of solid electrolytes is hindered by several challenges. These include poor compatibility at the electrode–electrolyte interface, low ionic conductivity at room temperature, and fast capacity degradation. To address these issues, here we propose ternary strategies by in-situ cross-linked plastic crystal electrolyte (in-situ PCE) based on succinonitrile (SN). Through the in-situ polymerization of SN with polyacrylonitrile/poly(vinylidene difluoride) (PAN/PVDF) nanofibers separator, excellent mechanical strength and compatibility at the electrode–electrolyte interface are achieved. The cross-linked structure of thermally polymerized ethoxylated trimethylolpropane triacrylate (ETPTA) immobilizes the SN molecule, preventing its contact with the lithium metal and inhibiting irreversible side reactions. Additionally, a LiF-rich passivation layer is employed to further protect the SN at the electrolyte-lithium metal interface. The dual protection from ETPTA and LiF offers excellent stability to lithium. Hence, the in-situ PCE exhibits high ionic conductivity (0.79 mS cm −1 at 30 °C) and wide electrochemical window (4.56 V, vs Li + /Li). The cells exhibit excellent cycling stability and high-rate performance. LiFePO 4 //Li cells retain 96.6 % capacity after 1000 cycles at 10C rate. This study provides valuable insights into the development of high-performance solid-state electrolytes.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 固态离子学
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ORGANIC ELECTRONICS · 2019 · IF 3.495

An inorganic hole-transport material of CuInSe2 for stable and efficient perovskite solar cells

Yan Zhang,Zhenlong Zhang,Yanyan Liu,Yuefeng Liu,Huiping Gao,Yanli Mao

In this work, we synthesized CuInSe 2 quantum dots (CISe QDs) and applied them to perovskite solar cells (PSCs) as an inorganic hole-transporting material (HTM). A power conversion efficiency (PCE) of 12.8% was achieved for the PSCs using CISe QDs as the HTM, which is the highest value reported to date for devices with a Cu-based chalcopyrite semiconductor as HTM. More importantly, the stability of PSCs with CISe QDs was significantly improved compared with that of the devices using spiro-OMeTAD as the HTM. These results demonstrate that CISe QDs are a promising inorganic HTM for PSCs with long-term stability and low cost.

研究领域: 材料科学 · 光伏技术 · 纳米材料 · 能源化学 · 半导体物理
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