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Passivating solid-electrolyte interphase (SEI) films arising from electrolytedecomposition on low-voltage lithium ion battery anode surfaces are criticalfor battery operations. We review the recent theoretical literature onelectrolyte decomposition and emphasize the modeling work on two-electronreduction of ethylene carbonate (EC, a key battery organic solvent). One of thetwo-electron pathways, which releases CO gas, is re-examined using simplequantum chemistry calculations. Excess electrons are shown to preferentiallyattack EC in the order (broken EC^-) > (intact EC^-) > EC. This confirms theviability of two electron processes and emphasizes that they need to beconsidered when interpreting SEI experiments. An estimate of the crossoverbetween one- and two-electron regimes under a homogeneous reaction zoneapproximation is proposed.

Two-electron reduction of ethylene carbonate: a quantum chemistry re-examination of mechanisms