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Published March 25, 2021 | Supplemental Material + Published
Journal Article Open

Effects of High and Low Salt Concentrations in Electrolytes at Lithium–Metal Anode Surfaces Using DFT-ReaxFF Hybrid Molecular Dynamics Method

Abstract

Due to creating a passivated solid electrolyte interphase (SEI), high concentration (HC) electrolytes demonstrate peculiar physicochemical properties and outstanding electrochemical performance. However, the structures of such SEI remains far from clear. In this work, a hybrid abinitio and reactive molecular dynamics (HAIR) scheme is employed to investigate the concentration effect of SEI formation by simulating the reductive degradation reactions of lithium bis(fluorosulfonyl)imide (LiFSI) in 1,3 dioxalane (DOL) electrolytes at concentrations of 1 M, 4 M, and 10 M. The efficient HAIR scheme allows the simulations to reach 1 ns to predict electrolytes' deep products at different concentrations. The simulation findings show that the most critical distinction between HC and its low concentration (LC) analogue is that anion decomposition in HC is much more incomplete when only S–F breaking is observed. These insights are important for the future development of advanced electrolytes by rational design of electrolytes.

Additional Information

© 2021 American Chemical Society. Received: February 5, 2021; Accepted: March 10, 2021; Published: March 16, 2021. T.C. and M.X. thanks the National Natural Science Foundation of China (Grants 21903058 and 22003044), the Natural Science Foundation of Jiangsu Higher Education Institutions (Grant SBK20190810), the Jiangsu Province High-Level Talents (Grant JNHB-106), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) for financial support. H.Y. thanks the China Postdoctoral Science Foundation (Grant 2019M660128) for financial support. This work was partly supported by the Collaborative Innovation Center of Suzhou Nano Science & Technology. The authors declare no competing financial interest.

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October 3, 2023
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