Volume 137, Issue 8 e202420411
Forschungsartikel

Coulombic Condensation of Liquefied Gas Electrolytes for Li Metal Batteries at Ambient Pressure

Yijie Yin

Yijie Yin

Program of Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093 USA

These authors contributed equally to this work.

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John Holoubek

John Holoubek

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

These authors contributed equally to this work.

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Kangwoon Kim

Kangwoon Kim

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Alex Liu

Alex Liu

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Bhargav Bhamwala

Bhargav Bhamwala

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Shen Wang

Shen Wang

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Bingyu Lu

Bingyu Lu

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Kunpeng Yu

Kunpeng Yu

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Hongpeng Gao

Hongpeng Gao

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Mingqian Li

Mingqian Li

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Ganesh Raghavendran

Ganesh Raghavendran

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Guorui Cai

Guorui Cai

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Weikang Li

Weikang Li

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

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Ping Liu

Ping Liu

Program of Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093 USA

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

Sustainable Power and Energy Center, University of California, San Diego, La Jolla, CA 92093 USA

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Ying Shirley Meng

Corresponding Author

Ying Shirley Meng

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

Sustainable Power and Energy Center, University of California, San Diego, La Jolla, CA 92093 USA

Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637 USA

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Zheng Chen

Corresponding Author

Zheng Chen

Program of Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093 USA

Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA 92093 USA

Sustainable Power and Energy Center, University of California, San Diego, La Jolla, CA 92093 USA

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First published: 09 December 2024

Abstract

The concept of employing highly concentrated electrolytes has been widely incorporated into electrolyte design, due to their enhanced Li-metal passivation and oxidative stability compared to their diluted counterparts. However, issues such as high viscosity and sub-optimal wettability, compromise their suitability for commercialization. In this study, we present a highly concentrated dimethyl ether-based electrolyte that appears as a liquid phase at ambient conditions via Li+ - solvents ion-dipole interactions (Coulombic condensation). Unlike conventional high salt concentration ether-based electrolytes, it demonstrates enhanced transport properties and fluidity. The anion-rich solvation structure also contributes to the formation of a LiF-rich salt-derived solid electrolyte interphase, facilitating stable Li metal cycling for over 1000 cycles at 0.5 mA cm−2, 1 mAh cm−2 condition. When combined with a sulfurized polyacrylonitrile (SPAN) electrode, the electrolyte effectively reduces the polysulfide shuttling effect and ensures stable performance across a range of charging currents, up to 6 mA cm−2. This research underscores a promising strategy for developing an anion-rich, high concentration ether electrolyte with decreased viscosity, which supports a Li metal anode with exceptional temperature durability and rapid charging capabilities.

Conflict of Interests

No potential competing interest was reported by the authors.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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