We review recent ab initio molecular dynamics studies ofelectrode/electrolyte interfaces in lithium ion batteries. Our goals are tointroduce experimentalists to simulation techniques applicable to models whichare arguably most faithful to experimental conditions so far, and to emphasizeto theorists that the inherently interdisciplinary nature of this subjectrequires bridging the gap between solid and liquid state perspectives. Weconsider liquid ethylene carbonate (EC) decomposition on lithium intercalatedgraphite, lithium metal, oxide-coated graphite, and spinel manganese oxidesurfaces. These calculations are put in the context of more widely studiedwater-solid interfaces. Our main themes include kinetically controlledtwo-electron-induced reactions, the breaking of a previously much neglectedchemical bond in EC, and electron tunneling. Future work on modeling batteriesat atomic lengthscales requires capabilities beyond state-of-the-art, whichemphasizes that applied battery research can and should drive fundamentalscience development.
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