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

Yue LiuQintao SunPeiping YuYu WuLiang XuHao YangMiao XieTao ChengWilliam A Goddard Iii
Published in: The journal of physical chemistry letters (2021)
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 ab initio 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.
Keyphrases
  • ionic liquid
  • molecular dynamics
  • ion batteries
  • solid state
  • density functional theory
  • simultaneous determination
  • gold nanoparticles
  • liquid chromatography
  • molecular docking
  • visible light
  • crystal structure