Highly Solvating Electrolytes for Lithium-Sulfur Batteries.,Advanced Energy Materials

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Highly Solvating Electrolytes for Lithium-Sulfur Batteries.
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2019-02-07 , DOI: 10.1002/aenm.201803096
Abhay Gupta ₁ , Amruth Bhargav ₁ , Arumugam Manthiram ₁

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There is a critical need to evaluate lithium-sulfur (Li-S) batteries with practically relevant high sulfur loadings and minimal electrolyte. Under such conditions, the concentration of soluble polysulfide intermediates in the electrolyte drastically increases, which can alter the fundamental nature of the solution-mediated discharge and thereby the total sulfur utilization. In this work, we present an investigation into various high donor number (DN) electrolytes that allow for increased polysulfide dissolution, and demonstrate how this property may in fact be necessary for increasing sulfur utilization at low electrolyte and high loading conditions. The solvents dimethylacetamide, dimethyl sulfoxide, and 1-methylimidazole are holistically evaluated against dimethoxyethane as electrolyte co-solvents in Li-S cells, and they are used to investigate chemical and electrochemical properties of polysulfide species at both dilute and practically relevant conditions. The nature of speciation exhibited by lithium polysulfides is found to vary significantly between these concentrations, particularly in regards to the S3 •- species. Furthermore, the extent of the instability in conventional electrolyte solvents and high DN solvents with both lithium metal and polysulfides is thoroughly investigated. These studies establish a basis for future efforts into rationally designing an optimal electrolyte for a lean electrolyte, high energy density Li-S battery.

中文翻译：

锂硫电池的高度溶剂化电解质。

迫切需要评估具有实际相关的高硫负载和最少电解质的锂硫（Li-S）电池。在这样的条件下，电解质中可溶性多硫化物中间体的浓度急剧增加，这可以改变溶液介导的放电的基本性质，从而改变总硫的利用率。在这项工作中，我们对允许增加多硫化物溶解的各种高给体数（DN）电解质进行了研究，并证明了在低电解质和高负荷条件下增加硫的利用率实际上可能是必需的。全面评估了溶剂二甲基乙酰胺，二甲基亚砜和1-甲基咪唑相对于Li-S电池中作为电解质助溶剂的二甲氧基乙烷，它们可用于研究在稀薄条件下和实际相关条件下多硫化物物种的化学和电化学性质。发现在这些浓度之间，多硫化锂所表现出的形态学性质差异很大，特别是在S3-物种方面。此外，彻底研究了常规电解质溶剂和高DN溶剂中锂金属和多硫化物的不稳定性程度。这些研究为将来为合理设计用于稀薄电解质，高能量密度Li-S电池的最佳电解质奠定了基础。发现在这些浓度之间，多硫化锂所表现出的形态学性质差异很大，特别是在S3-物种方面。此外，彻底研究了常规电解质溶剂和高DN溶剂中锂金属和多硫化物的不稳定性程度。这些研究为将来为合理设计用于稀薄电解质，高能量密度Li-S电池的最佳电解质奠定了基础。发现在这些浓度之间，多硫化锂所表现出的形态学性质差异很大，特别是在S3-物种方面。此外，彻底研究了常规电解质溶剂和高DN溶剂中锂金属和多硫化物的不稳定性程度。这些研究为将来为合理设计用于稀薄电解质，高能量密度Li-S电池的最佳电解质奠定了基础。

更新日期：2018-12-13

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