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通过湿法工艺制备锂金属电极的人工固体电解质界面:金属盐浓度和溶剂选择的作用

Artificial Solid Electrolyte Interphases for Lithium Metal Electrodes by Wet Processing: The Role of Metal Salt Concentration and Solvent Choice.

作者信息

Thanner Katharina, Varzi Alberto, Buchholz Daniel, Sedlmaier Stefan J, Passerini Stefano

机构信息

Helmholtz Institute Ulm (HIU), Helmholtzstraße 11, 89081 Ulm, Germany.

Karlsruhe Institute of Technology (KIT), P.O.Box 3640, 76021 Karlsruhe, Germany.

出版信息

ACS Appl Mater Interfaces. 2020 Jul 22;12(29):32851-32862. doi: 10.1021/acsami.0c08938. Epub 2020 Jul 13.

Abstract

In this study, the artificial solid electrolyte interphase (SEI) formed on lithium metal when treated in ZnCl solutions is thoroughly investigated. The artificial SEI on lithium metal electrodes substantially decreases the interfacial resistance by ca. 80% and improves cycling stability in comparison to untreated lithium. The presence of a native SEI negatively affects the morphology and interfacial resistance of the artificial SEI. Increasing the ZnCl concentration in tetrahydrofuran (THF) (precursor solution) results in higher homogeneity of the surface morphology. Independent of the ZnCl concentrations, the artificial SEI is composed of C, CO, LiCl, LiCO, ZnCl, and LiZn alloys. ZnCl (1 M) produces the most homogenous surface and additional surface species with carbonyl side groups. Nonetheless, the ZnCl concentration only has a small effect on the interfacial resistance or cycling stability. Using ethyl methyl carbonate (EMC) as the solvent significantly reduces the interfacial resistance to 7 Ω cm, in comparison to 25 Ω cm for THF. The composition of the artificial SEIs varies depending on the solvent. Either way, the SEI consists of C LiC, LiCl, LiCO, ZnCl, and LiZn alloys. The THF-based SEI additionally features ether and carbonyl groups, LiZnO, and Zn metal. For the artificial SEI formed with both solvents, the atomic percentage of the LiZn alloy increases close to the Li surface.

摘要

在本研究中,对锂金属在ZnCl溶液中处理时形成的人工固体电解质界面(SEI)进行了深入研究。与未处理的锂相比,锂金属电极上的人工SEI使界面电阻大幅降低约80%,并提高了循环稳定性。原生SEI的存在对人工SEI的形态和界面电阻产生负面影响。增加四氢呋喃(THF)(前驱体溶液)中ZnCl的浓度会导致表面形态具有更高的均匀性。与ZnCl浓度无关,人工SEI由C、CO、LiCl、LiCO、ZnCl和LiZn合金组成。1 M的ZnCl产生最均匀的表面以及带有羰基侧基的额外表面物种。尽管如此,ZnCl浓度对界面电阻或循环稳定性的影响很小。与THF的25 Ω·cm相比,使用碳酸甲乙酯(EMC)作为溶剂可将界面电阻显著降低至7 Ω·cm。人工SEI的组成因溶剂而异。无论哪种方式,SEI都由C、LiC、LiCl、LiCO、ZnCl和LiZn合金组成。基于THF的SEI还具有醚基和羰基、LiZnO以及Zn金属。对于用两种溶剂形成的人工SEI,LiZn合金的原子百分比在靠近Li表面处增加。

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