Effects of charged interfaces on electrolyte decomposition at the lithium metal anode

Camacho-Forero, Luis E.; Balbuena, Perla B.

doi:10.1016/j.jpowsour.2020.228449

Title: Effects of charged interfaces on electrolyte decomposition at the lithium metal anode

Journal Article · Sat Jul 04 00:00:00 EDT 2020 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2020.228449· OSTI ID:1838877

Camacho-Forero, Luis E. ^[1]; Balbuena, Perla B. ^[1]

Texas A & M Univ., College Station, TX (United States)

Lithium–Sulfur batteries are promising candidates to substitute conventional Li-ion batteries due to their higher energy density and reduced cost. However, several challenges related to the reactivity of the lithium metal anode have prevented this technology from becoming broadly commercialized. Lithium's high reactive nature leads to the continuous decomposition of the electrolyte and the formation of the solid-electrolyte interphase (SEI) layer. Thus, a comprehensive understanding of how the SEI film is formed is crucial to help elucidate improvements for this battery technology. In this work, we use density functional theory (DFT) based computational methods to investigate the effect of charged interfaces on the electrolyte degradation at the lithium anode. Here, several electrolyte mixtures were considered including 1,2-dimethoxyethane (DME) and 1,3-dioxolane (DOL) as solvents, and lithium bis(fluorosulfonyl)imide (LiFSI) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as salts. It is found that the extent of salt decomposition is higher when the interface is charged. In addition, two types of solvent reduction mechanisms are identified: C–O bond cleavage and radical attacks. Charge transfer and evolution analysis are characterized in detail. Finally, solvent decomposition reactions are found to become more thermodynamically favorable and their activation barriers to be diminished under the effect of constant potentials and electric fields.

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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); USDOE Office of Science (SC)

Grant/Contract Number:: EE0008210; AC02-05CH11231

OSTI ID:: 1838877

Alternate ID(s):: OSTI ID: 1637366

Journal Information:: Journal of Power Sources, Vol. 472; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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