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Issue 3, 2015
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Predicting the voltage dependence of interfacial electrochemical processes at lithium-intercalated graphite edge planes

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Abstract

The applied potential governs lithium-intercalation and electrode passivation reactions in lithium ion batteries, but are challenging to calibrate in condensed phase DFT calculations. In this work, the “anode potential” of charge-neutral lithium-intercalated graphite (LiC6) with oxidized edge planes is computed as a function of Li-content (nLi) at edge planes, using ab initio molecular dynamics (AIMD), a previously introduced Li+ transfer free energy method, and the experimental Li+/Li(s) value as reference. The voltage assignments are corroborated using explicit electron transfer from fluoroethylene carbonate radical anion markers. PF6 is shown to decompose electrochemically (i.e., not just thermally) at low potentials imposed by our voltage calibration technique. We demonstrate that excess electrons reside in localized states-in-the-gap in the organic carbonate liquid region, which is not semiconductor-like (band-state-like) as widely assumed in the literature.

Graphical abstract: Predicting the voltage dependence of interfacial electrochemical processes at lithium-intercalated graphite edge planes

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Publication details

The article was received on 05 Oct 2014, accepted on 06 Nov 2014 and first published on 21 Nov 2014


Article type: Paper
DOI: 10.1039/C4CP04494K
Citation: Phys. Chem. Chem. Phys., 2015,17, 1637-1643
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    Predicting the voltage dependence of interfacial electrochemical processes at lithium-intercalated graphite edge planes

    K. Leung, Phys. Chem. Chem. Phys., 2015, 17, 1637
    DOI: 10.1039/C4CP04494K

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