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CHEMICAL ENGINEERING SCIENCE · 2019 · IF 3.372

A sandwich-structured double-battery device for direct evaluation of lithium diffusion coefficients and phase transition in electrodes of lithium ion batteries

Kechun Wen,Mingfu Xia,Pan Deng,Weiqiang Lv,Weidong He

Li diffusion efficiency reflects the kinetics of Li intercalation/de-intercalation in solid electrode materials and determines the rate performances of Li ion batteries. Traditional techniques including the electrochemical impedance spectroscopy, potential intermittent titration technique, potential relaxation technique, galvanostatic intermittent titration technique, and cyclic voltammetry, could lead to significant disagreement on Li chemical diffusion coefficients due to the limited reliability of the parameters required for calculating Li diffusion coefficients. Based on the Nernst-Einstein equation, a double-battery system is proposed for the direct measurement of chemical diffusion coefficients of Li in solid electrodes. With the double-battery system, Li diffusion coefficients in the intercalation/de-intercalation of graphite electrodes featured with phase-transition and double-phase regions, are measured efficiently, with consistent values in the range of 10 −10 –10 −9  cm 2 /s. The direct measurement then allows for the evaluation of the diffusion barrier associated with Li intercalation/de-intercalation in the electrodes.

研究领域: 电化学 · 材料科学 · 能源存储 · 固态离子学 · 电池技术
✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Recovery Li/Co from spent LiCoO2 electrode based on an aqueous dual-ion lithium-air battery

Yu Zhou,Wei Shan,Shaofeng Wang,Kwok-ho Lam,Qiang Ru,Fuming Chen,Xianhua Hou

While lithium-ion batteries dominate the field of electronic devices and vehicles, recovery of LiCoO 2 from spent batteries becomes a significant process. Aqueous lithium-air battery and dual-ion battery were blended into a novel electrochemical system as dual-ion lithium-air battery (DLAB) system to recover Li and Co elements from the spent LiCoO 2 (acid solution). In the system, oxygen, LiCoO 2 acid solution and Li 2 Ti 2 (PO 4 ) 3 (LTPO), which has Na + superionic conductor structure and is synthesized by sol-gel method, were used as cathode, dual-ion electrolyte and anode. Relatively low voltage plateaus, stability and insolubility of LTPO make it to be a feasible candidate for this aqueous DLAB. By applying Pt/C as a catalyst for cathode, the full discharged system exhibits a Co ion recovering rate of up to 96.2%. Moreover, this system presents positive discharge plateaus at around 0.47 V and 0.10 V during recovering, demonstrating an output energy density of 43.88 Wh kg −1 . The system shows a green and promising way for the recovery of spent LiCoO 2 battery.

研究领域: 电化学 · 能源材料 · 环境工程 · 电池回收 · 无机化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Polyimide-reinforced solid polymer electrolyte with outstanding lithium transferability for durable Li metal batteries

Yuhong Ma,Yu Jiao,Yichao Yan,Wei Chen,Yaoyao Li,Mingjie Zhou,Dongjiang Chen,Jun Zhu

Solid polymer electrolytes drastically enhance the operational safety of Li metal battery by eliminating the flammable liquid electrolyte, but still suffer from low ionic conductivity and inferior thermostability. Herein, we tack this issue by strengthening the polyvinylidene fluoride matrix with lithiophilic polyimide . The actively conjugated carbonyl groups in polyimide polymer backbone with Li + -conductivity feature accelerate the ion conduction, accordingly improving the ionic conductivity up to 4.1 × 10 −4  S cm −1 . With the polyimide solid electrolyte , lithium symmetrical battery shows a stable operation without obvious dendrite growth over 300 h at 0.17 mA cm −2 , effectively uniformizing the Li + deposition at the electrolyte/anode interface. The LiFePO 4 cell based on the polyimide electrolyte delivers a high discharge capacity of 126 mAh g −1 at 25 °C with a capacity retention of 86% after 500 cycles at 0.15 mA cm −2 . In addition, polyimide chain with high thermostability owns affinity to polyvinylidene fluoride with an adsorption energy of 0.1 eV, giving rise to 35% enhancement in mechanical strength and 68% reduction in thermal shrinkage at 300 °C as compared with pure polyvinylidene fluoride electrolyte. This design allows a promising route for enhancing the safety operation of polymer electrolyte and promoting ionic transfer by reconstructing the polymer architecture .

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

NaClO4 as an effective electrolyte additive for high-energy Li-ion batteries

Yi-Xuan Li,Xiang Ding,Fei Chen,Kuo Cao,Chun-Hua Chen

NaClO 4 is utilized as a salt-type electrolyte additive to improve the electrochemical performance in both Li-rich/graphite full cells and Li-rich/Li half cells. The corresponding characterizations such as scanning electron microscopy and X-ray photoelectron spectroscopy reveal that the NaClO 4 -added electrolyte can suppress the transition metal dissolution from Li-rich cathode and form a stable conductive cathode electrolyte interface layer to protect Li-rich cathode and promote Li + ions transfer. A small amount (0.1 wt%) of NaClO 4 additive enables Li-rich/graphite full cells to maintain 86% capacity after 50 cycles and Li-rich/Li half cells to maintain 95% capacity after 100 cycles, showing a great application potential.

研究领域: 电化学 · 材料科学 · 能源存储 · 电池技术 · 功能材料
✓ 已验证 DOI 高影响因子
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MATERIALS CHEMISTRY AND PHYSICS · 2019 · IF 2.781

Achieving superior electrochemical performances on LiNi0.8Co0.15Al0.05O2 cathode materials by cadmium oxide modification

Yunjiao Li,Shilei Wang,Yongxiang Chen,Tongxing Lei,Shiyi Deng,Jie Zhu,Jinping Zhang,Jia Guo

Cadmium oxides (CdO), an important semiconductor material , have many superior properties when used as a cathode material for nickel-cadmium batteries. Here, the coating and the doped co-modified LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode are constructed by a continuous wet chemical process and a high-temperature sintering process, wherein the Cd 2+ are uniformly doped in a gradient form and the CdO protective layer is distributed on the outer surface of secondary particles. The Cd-modified NCA material has more stable interfacial and crystal lattice structure, thereby inhibiting harmful phase transitions and side-reactions. Accordingly, the modified sample has excellent electrochemical performance and maintaining a complete spherical morphology during long cycling compared to the pristine sample. In addition, as a pillar ion, cadmium increases the plate spacing and lithium-ion diffusion kinetics. The electrochemical results show that the capacity retention of the modified sample Cd-2000 reached 96.5% and 90.6% after 100 cycles and 200 cycles respectively at 1 C. At the high current rate of 8 C, the initial capacity and retention (100 cycles, 3.0–4.3 V) reach 166.2 mAh g −1 and 95.2%, respectively. Besides, the results of electrochemical impedance spectroscopy (EIS) reveal that CdO modification could decrease the resistance of the cell polarization and impedance increment upon cycling.

研究领域: 材料科学 · 电化学 · 能源存储 · 无机化学 · 半导体材料
✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2020 ·Vol. 46 ·期 8 ·10917-10924 · IF 3.83

Rapid sintering method for highly conductive Li7La3Zr2O12 ceramic electrolyte

Li Yang,Qiushi Dai,Lei Liu,Dingsheng Shao,Kaili Luo,Sidra Jamil,Hong Liu,Zhigao Luo,Baobao Chang,Xianyou Wang

Solid electrolytes could address the increasingly urgent safety and energy density concerns of lithium-ion batteries. Among several kinds of solid electrolytes, Ta-doped Li 7 La 3 Zr 2 O 12 (Ta-LLZO) became a research hotspot because of its high Li-ion conductivity and chemical stability against Li-metal and air. However, the preparation of high quality LLZO ceramic electrolyte via conventional air ambient sintering method is still a big challenge due to the serious “Li-loss” and abnormal grain growth phenomenon during the long-time high-temperature sintering process . Herein, a new rapid ultra-high-temperature air ambient sintering method without mother powder (MP) is put forward for the preparation of high quality Ta-LLZO ceramic electrolyte. The rapid sintering strategy can effectively restrain “Li-loss”. Furthermore, it is demonstrated that the none-mother-powder method is superior to traditional mother-powder method. Ta-LLZO ceramics sintered without MP via this rapid sintering method own small grain size, tight grain boundary, dense microstructure and high conductivity. Specifically, the Ta-LLZO ceramic sintered at 1360 °C for 10 min without MP exhibits high conductivity (8.5 × 10 −4  S cm −1 at 25 °C) and high relative density (97%), which equate those made by hot pressing sintering method. Without MP, the sintering process can avoid a lot of material waste and simplify the operation process. Moreover, the rapid sintering process can sharply shorten sintering time and reduce energy consumption. Therefore, this low-cost high-efficient sintering strategy can be effectively used in the large-scale production of high-quality Ta-LLZO ceramic electrolyte.

研究领域: 材料科学 · 固态离子学 · 能源材料 · 电化学 · 无机非金属材料 · 电池技术
✓ 已验证 DOI 高影响因子
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Carbon Neutrality · 2023 ·Vol. 2 ·期 1 ·1-11 · IF 0

Understanding steric hindrance effect of solvent molecule in localized high-concentration electrolyte for lithium metal batteries

Li Xinpeng,Pan Yuxue,Liu Yue,Jie Yulin,Chen Shunqiang,Wang Shiyang,He Zixu,Ren Xiaodi,Cheng Tao,Cao Ruiguo,Jiao Shuhong

High energy density lithium metal batteries (LMBs) have garnered significant research interests in the past decades. However, the growth of lithium dendrites and the low Coulombic efficiency (CE) of Li metal anode pose significant challenges for the development of LMBs. Herein, we report a triethyl orthoformate (TEOF)-based localized high-concentration electrolyte (LHCE) that facilitates a highly reversible Li metal anode with dendrite-free deposition morphologies and an average Coulombic efficiency of 99.1% for 450 cycles. Mechanistic study reveal that the steric hindrance caused by the terminal ethyl groups in the TEOF solvent molecule results in a weak solvating ability, leading to the formation of anion-dominant solvation structures. The anion-dominant solvation sheaths play an essential role in the formation of a LiF-rich solid-electrolyte interphase (SEI), which effectively suppresses the growth of Li dendrites. Furthermore, the TEOF-based electrolyte demonstrates the stable cycling of high-voltage Li||NMC811 cells. These results provide insights into understanding of steric hindrance effect on electrolyte solvation structure and offer valuable guidance for the design of electrolyte solvents in the development of lithium metal batteries.

研究领域: 电化学储能 · 材料科学 · 能源化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Regulating and understanding the compatibility of sulfide composite solid-state electrolyte in nickel-rich lithium metal batteries

Haoyang Yuan,Changhao Tian,Mengyuan Song,Wenjun Lin,Tao Huang,Aishui Yu

In the pursuit of high-energy-density lithium batteries, composite solid-state electrolytes are highly favored due to the combination of flexibility and acceptable ionic conductivity. However, challenges such as unpredictable lithium dendrite growth, cathode material structural instability, and oxidative resistance at high voltages pose significant hurdles for solid-state batteries. To investigate the synergistic interactions of polymers and sulfides, a hybrid poly (1,3-dioxolane) and poly (polyethylene glycol diacrylate) blend was designed through in-situ polymerization, allowing LiFePO 4 //Li batteries to achieve an average coulombic efficiency exceeding 99% at 0.5C and stable cycling for at least 1000 h in lithium symmetric cells. Computational analysis and component detection demonstrate the stability of the components and the formation of a LiF-stabilized anode from lithium salt decomposition. Similarly, on the cathode side, when Li 3 PO 4 -coated LiNi 0.6 Co 0.2 Mn 0.2 O 2 is used as the cathode material, a more stable interface suppresses cathode particles' collapse and harmful electrolytes’ decomposition. In ambient environments, after 200 cycles at 0.5C, the capacity retention remains as high as 90.48%. Impedance changes by in-situ methods and component composition were further analyzed. This work integrates multiple methods and stabilizes and validates the anode and cathode interface, providing a promising approach and strategy for designing high-performance sulfide composite solid-state batteries.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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RSC Advances · 2015 ·Vol. 5 ·期 86 ·70527-70535 · IF 3.84

A novel shuttle-like Fe3O4–Co3O4 self-assembling architecture with highly reversible lithium storage

Kaina Shang,Wentao Li,Yongmei Liu,Wenguang Zhang,Hui Yang,Jiqing Xie,Zuyan Liu,Shu-Lei Chou,Lingzhi Zhao,Ronghua Zeng

We report the synthesis of a novel shuttle-like Fe3O4–Co3O4 self-assembling architecture through a facile hydrothermal method. The composite manifests quite excellent electrochemical performance as anodes of Li-ion batteries. It delivers a high reversible capacity of ∼1013 mA h g−1 at 100 mA g−1 after 100 cycles (∼1246 mA h g−1 at 0.5 A g−1, 864 mA h g−1 at 1 A g−1 and 625 mA h g−1 at 2 A g−1 after 50 cycles). The rate performance is also outstanding with a reversible capacity of 660 mA h g−1 even at 5 A g−1 and a capacity retention of 94% after 78 cycles. The synergetic effect of Co3O4 and Fe3O4, as well as the unique self-assembling architecture, may be responsible for the large enhanced electrochemical performance.

研究领域: 材料科学 · 电化学 · 纳米材料 · 能源存储 · 锂离子电池
✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Insight into the effect of lithium-dendrite suppression by lithium bis(fluorosulfony)imide/1,2-dimethoxyethane electrolytes

Peng Zhang,Han Jin,Tong Wang,Miao Wang

The highly concentrated lithium bis(fluorosulfonyl)imide/1,2–dimethoxyethane electrolyte is in the good graces of researchers due to its excellent electrochemical performance in lithium-metal batteries. However, our study reveals that the more concentrated electrolyte incurred more drastic lithium-dendrite growth. Minimum onset time (t sc ) of lithium-dendrite formation of only 7.4 and 18.6 h are observed in 4 M lithium bis(fluorosulfonyl)imide/1,2-dimethoxyethane electrolyte galvanostatically polarized at current densities of 1.0 and 0.5 mA cm −2 , respectively. In contrast, t sc are as long as around 56 and > 190 h in 1 M electrolyte at 1.0 and 0.5 mA cm −2 , respectively. We found that 1 M electrolyte has comprehensive advantages in many respects, including Li + transference number (0.61), salt diffusion coefficient (1.47 × 10 −5  cm 2  s −1 ), ionic conductivity (1.52 × 10 −2  S cm −1 ), low polarization potential and solid electrolyte interphase protection, which collectively make contributions to outstanding lithium-dendrite suppression.

研究领域: 电化学 · 材料科学 · 能源存储 · 电池技术 · 界面化学
✓ 已验证 DOI 高影响因子
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IONICS · 2016 ·Vol. 23 ·期 3 ·575-583 · IF 2.119

Advanced LiTi2(PO4)3/C anode by incorporation of carbon nanotubes for aqueous lithium-ion batteries

He Zhangxing,Jiang Yifan,Sun Dan,Dai Lei,Wang Haiyan

Inferior rate capability is a big challenge for LiTi 2 (PO 4 ) 3 anode for aqueous lithium-ion batteries. Herein, to address such issue, we synthesized a high-performance LiTi 2 (PO 4 ) 3 /carbon/carbon nanotube (LTP/C/CNT) composite by virtue of high-quality carbon coating and incorporation of good conductive network. The as-prepared LTP/C/CNT composite exhibits excellent rate performance with discharge capacity of 80.1 and 59.1 mAh g −1 at 10 C and 20 C (based on the mass of anode, 1 C = 150 mA g −1 ), much larger than that of the LTP/C composite (53.4 mAh g −1 at 10 C, and 31.7 mAh g −1 at 20 C). LTP/C/CNT also demonstrates outstanding cycling stability with capacity retention of 83.3 % after 1000 cycles at 5 C, superior to LTP/C without incorporation of CNTs (60.1 %). As verified, the excellent electrochemical performance of the LTP/C/CNT composite is attributed to the enhanced electrical conductivity, rapid charge transfer, and Li-ion diffusion because of the incorporation of CNTs.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2021 · IF 4.464

Preparation and performances of poly (ethylene oxide)-Li6PS5Cl composite polymer electrolyte for all-solid-state lithium batteries

Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Zhigao Luo,Xianyou Wang

Composite polymer electrolytes (CPEs), which are made up of sulfide solid electrolyte Li 6 PS 5 Cl dispersed in solid polymer electrolytes (SPEs) based on the poly (ethylene oxide) (PEO), has been prepared by adopting solution casting method. The results show that the addition of appropriate amount of Li 6 PS 5 Cl can enhance lithium-ion conductivity and interfacial stability of solid polymer electrolyte, which can play an active role in the electrochemical properties of the improving all-solid-state LiFePO 4 /Li batteries. Especially, the PEO-1 wt% Li 6 PS 5 Cl exhibits a high lithium-ion conductivity of 8.84 × 10 −4 S/cm at 80 ℃ and 7.58 × 10 −5 S/cm at 30 ℃. Compared with the SPE, the PEO-1 wt% Li 6 PS 5 Cl has smaller interfacial impedance and more stable interface with lithium metal. Therefore, all-solid-state LiFePO 4 /Li batteries assembled by the PEO-1 wt% Li 6 PS 5 Cl represent higher coulomb efficiency, and better cycle stability with high initial discharge capacity of 155.43 mAh/g, 134.95 mAh/g at current rates of 0.2C, 0.5C at 60 ℃, respectively.

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
✓ 已验证 DOI 高影响因子
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