Electric double layer studies of Li electrode—PEO-LiTFSI electrolyte by constant potential simulations
File(s)
Supporting information
Author(s)
Gullbrekken, Ø
Bresme, F
Selbach, SM
Schnell, SK
Type
Journal Article
Abstract
Electrochemical interfaces are highly complex, but important to understand to enable new and better battery technologies. Here, the structure and transport properties of the interface between Li metal and PEO-LiTFSI polymer electrolyte, including the electric double layer, are investigated by density functional theory computations and molecular dynamics simulations. Significant charge transfer is observed for a neutral short PEO chain when approaching the Li surface. The interfaces next to the negative and positive electrodes are different; the negative interface is being dominated by the polymer and Li+, while the anions make up more of the positive interface. Adsorption of Li+ ions on the Li slab is observed at high salt concentrations (0.98–3.56 mol L−1) and potential differences (0–4 V). The adsorption energy of the Li+ ions at the interface does not correlate with the Li+ transport kinetics, which is very slow, particularly next to the negative electrode. Slow interface kinetics might contribute to slow charge transfer and non-uniform Li plating. The adsorption of Li+ is only slightly affected by the electric potential difference between the electrodes.
Date Issued
2026-02-21
Date Acceptance
2026-01-30
Citation
Journal of Chemical Physics, 2026, 164 (7)
ISSN
0021-9606
Publisher
American Institute of Physics
Journal / Book Title
Journal of Chemical Physics
Volume
164
Issue
7
Copyright Statement
Copyright © 2026 Author(s). This is the author’s accepted manuscript made available under a CC-BY licence in accordance with Imperial’s Research Publications Open Access policy (www.imperial.ac.uk/oa-policy)
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/41717968
PII: 3380544
Publication Status
Published
Coverage Spatial
United States
Article Number
074708
Date Publish Online
2026-02-20