Anionic Effects on Li-Ion Transport and Electrochemical Properties of High-Concentration Li Salt/Sulfone Electrolytes

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Yosuke Ugata, Shuhei Miyazaki, Gakuto Wada, Shohei Sasagawa and Kaoru Dokko*, 
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Abstract

High-concentration electrolytes (HCEs) comprising Li salts and sulfones are regarded as promising materials for boosting the thermal stability, energy density, and rate capability of Li batteries. In this study, to obtain a deeper understanding of the correlation between electrolyte composition and physicochemical properties, the anionic effects in binary mixtures of various Li salts and 3-methylsulfolane (MSL) were systematically studied. The ionic conductivity of the Li salt/MSL mixtures increased as the Lewis basicity of the anions becomes weaker. In HCEs with a molar ratio of Li salt/MSL = 1/4, the fraction of free MSL decreased as the Lewis basicity of the anions weakened, leading to a higher activity of Li+. The Li ion transference number in the HCEs decreased with weakening of the Lewis basicity of the anion. Electrochemical impedance measurements revealed that the charge-transfer kinetics of the LiCoO2 and Li metal electrodes in the HCEs were enhanced using weaker Lewis basic anions. Our findings reveal that the utilization of Li salts with weak Lewis basic anions is essential for enhancing the power density of lithium batteries with HCEs. This work provides insights into the functions of anions in sulfone-based HCEs and the correlation between the HCE composition and battery performance, which may be helpful for the design of electrolytes of advanced lithium batteries.

Abstract Image

阴离子对高浓度锂盐/砜电解质锂离子输运及电化学性能的影响
含有锂盐和砜的高浓度电解质(HCEs)被认为是提高锂电池热稳定性、能量密度和倍率能力的有前途的材料。为了更深入地了解电解质组成与理化性质之间的关系,本研究系统地研究了不同锂盐与3-甲基亚砜(MSL)二元混合物中的阴离子效应。锂盐/MSL混合物的离子电导率随着阴离子路易斯碱度的减弱而增大。在Li盐/MSL摩尔比为1/4的HCEs中,随着阴离子路易斯碱度的减弱,游离MSL的比例降低,导致Li+活性升高。随着阴离子路易斯碱度的减弱,hce中Li离子的转移数减少。电化学阻抗测量结果表明,使用较弱的路易斯碱性阴离子可以增强hce中LiCoO2和Li金属电极的电荷转移动力学。研究结果表明,利用具有弱Lewis碱性阴离子的Li盐对于提高hce锂电池的功率密度至关重要。本研究揭示了阴离子在砜基HCE中的作用,以及HCE组成与电池性能之间的关系,对先进锂电池电解质的设计有一定的指导意义。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
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