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Enhanced Cycling Stability of Rechargeable Li-O-2 Batteries Using High-Concentration Electrolytes

机译:使用高浓度电解质增强可充电Li-O-2电池的循环稳定性

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摘要

The stability of electrolytes against highly reactive, reduced oxygen species is crucial for the development of rechargeable Li-O-2 batteries. In this work, the effect of lithium salt concentration in 1,2-dimethoxyethane (DME)-based electrolytes on the cycling stability of Li-O-2 batteries is investigated systematically. Cells with highly concentrated electrolyte demonstrate greatly enhanced cycling stability under both full discharge/charge (2.0-4.5 V vs Li/Li+) and the capacity-limited (at 1000 mAh g(-1)) conditions. These cells also exhibit much less reaction residue on the charged air-electrode surface and much less corrosion of the Li-metal anode. Density functional theory calculations are used to calculate molecular orbital energies of the electrolyte components and Gibbs activation energy barriers for the superoxide radical anion in the DME solvent and Li+-(DME) (n) solvates. In a highly concentrated electrolyte, all DME molecules are coordinated with salt cations, and the C-H bond scission of the DME molecule becomes more difficult. Therefore, the decomposition of the highly concentrated electrolyte can be mitigated, and both air cathodes and Li-metal anodes exhibit much better reversibility, resulting in improved cyclability of Li-O-2 batteries.
机译:电解质对高反应性,减少的氧种类的稳定性对于可充电Li-O-2电池的开发至关重要。在这项工作中,系统地研究了1,2-二甲氧基乙烷(DME)基电解质中锂盐浓度对Li-O-2电池循环稳定性的影响。具有高浓度电解质的电池在完全放电/充电(相对于Li / Li +为2.0-4.5 V)和容量受限(在1000 mAh g(-1)下)条件下都表现出大大增强的循环稳定性。这些电池在带电的空气电极表面上还表现出更少的反应残留物,并且对锂金属阳极的腐蚀也更少。密度泛函理论计算用于计算DME溶剂和Li +-(DME)(n)溶剂化物中超氧化物自由基阴离子的电解质组分的分子轨道能和Gibbs活化能垒。在高度浓缩的电解质中,所有DME分子均与盐阳离子配位,并且DME分子的C-H键断裂变得更加困难。因此,可以减轻高浓度电解质的分解,并且空气阴极和锂金属阳极都表现出更好的可逆性,从而改善了Li-O-2电池的循环能力。

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  • 来源
    《Advanced Functional Materials》 |2016年第4期|605-613|共9页
  • 作者单位

    Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99354 USA|Beijing Univ Chem Technol, Dept Chem Engn, Beijing 100029, Peoples R China;

    Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA;

    US Army, Res Lab, Sensors & Elect Devices Directorate, Power & Energy Div, Adelphi, MD 20783 USA;

    Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99354 USA;

    Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99354 USA;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    air electrodes; high-concentration electrolytes; Li-O-2 batteries; lithium metal; stability;

    机译:空气电极;高浓度电解质;Li-O-2电池;金属锂;稳定性;

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