Simulation guided molecular design of hydrofluoroether solvent for high energy batteries

Zhou Yu, Zhangxing Shi, Sambasiva R. Bheemireddy, Ethan Kamphaus, Xingyi Lyu, Mohammad Afsar Uddin, Zhiguang Li, Zhenzhen Yang, Tao Li, Jeffrey S. Moore, Lu Zhang, Lei Cheng

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Electrolyte design is critical for enabling next-generation batteries with higher energy densities. Hydrofluoroether (HFE) solvents have drawn a lot of attention as the electrolytes based on HFEs showed great promise to deliver highly desired properties, including high oxidative stability, ionic conductivity, as well as enhanced lithium metal compatibility. However, the solvation-property relationships and design principles for high-performance HFE solvents are still poorly understood. Herein, we proposed four novel asymmetric HFE designs by systematically varying polyether and fluorocarbon structural building blocks. By leveraging molecular dynamics (MD) modeling to analyze the solvation structures and predict the properties of the corresponding 1 M lithium bis(fluorosulfonyl)imide (LiTFSI) solutions, we downselected the most promising candidate based on high conductivity, solvation species distribution, and oxidative stability for extensive electrochemical characterizations. The formulated electrolyte demonstrated properties consistent with the predictions from the simulations and showed much-improved capacity retention as well as coulombic efficiency compared to the baseline electrolytes when cycled in lithium metal cells. This work exemplifies the construction of candidate electrolytes from building block functional moieties to engineer fundamental solvation structures for desired electrolyte properties and guide the discovery and rational design of new solvent materials.

Original languageEnglish
Pages (from-to)6294-6301
Number of pages8
JournalJournal of Materials Chemistry A
Volume12
Issue number11
DOIs
StatePublished - Feb 12 2024
Externally publishedYes

Funding

This research was supported by the Joint Center for Energy Storage Research (JCESR), a U.S. Department of Energy, Energy Innovation Hub. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (\u201CArgonne\u201D). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under contract no. DE-AC02-06CH11357. We gratefully acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. The authors thank Dr Kang Xu, Dr Marshall Schroeder and Dr Janet Ho from Army Research Laboratory for inspiring discussions regarding the characterization of electrolyte behavior on lithium metal surfaces. T. Li is thankful for the assistance from Bowen An at Northern Illinois University.

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