Liquid state properties of SEI components in dimethoxyethane

Journal Article · Wed Sep 22 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0059246· OSTI ID:1838689

Kamphaus, Ethan P. ^[1]; Balbuena, Perla B. ^[2]

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1. Texas A & M Univ., College Station, TX (United States); Texas A&M University
2. Texas A & M Univ., College Station, TX (United States)

The solid-electrolyte interphase (SEI) layer is a critical constituent of battery technology, which incorporates the use of lithium metals. Since the formation of the SEI is difficult to avoid, the engineering and harnessing of the SEI are absolutely critical to advancing energy storage. One problem is that much fundamental information about SEI properties is lacking due to the difficulty in probing a chemically complex interfacial system. One such property that is currently unknown is the dissolution of the SEI. This process can have significant effects on the stability of the SEI, which is critical to battery performance but is difficult to probe experimentally. Here, we report the use of ab initio computational chemistry simulations to probe the solution state properties of SEI components LiF, Li₂O, LiOH, and Li₂CO₃ in order to study their dissolution and other solution-based characteristics. Ab initio molecular dynamics was used to study the solvation structures of the SEI with a combination of radial distribution functions, discrete solvation structure maps, and vibrational density of states, which allows for the determination of free energies. From the change in free energy of dissolution, we determined that LiOH is the most likely component to dissolve in the electrolyte followed by LiF, Li₂CO₃, and Li₂O although none were favored thermodynamically. Furthermore, this indicates that dissolution is not probable, but Li₂O would make the most stable SEI with regard to dissolution in the electrolyte.

• Research Organization: Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE)
• Grant/Contract Number: EE0008210
• OSTI ID: 1838689
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 12 Vol. 155; ISSN 0021-9606
• Publisher: American Institute of Physics (AIP)
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ab-initio molecular dynamics
batteries
classical statistical mechanics
computational chemistry
density of states
electrolytes
energy storage
interphases
solvation
vibrational spectra