Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries

• Published in: Journal of physical chemistry. C Vol. 117; no. 4; pp. 1539 - 1547
• Main Author: Leung, Kevin
• Format: Journal Article
• Language: English
• Published: Columbus, OH American Chemical Society 31.01.2013
• Subjects: Applied sciences; Condensed matter: structure, mechanical and thermal properties; Diffusion; interface formation; Direct energy conversion and energy accumulation; Electrical engineering. Electrical power engineering; Electrical power engineering; Electrochemical conversion: primary and secondary batteries, fuel cells; Exact sciences and technology; Physics; Solid surfaces and solid-solid interfaces; Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties); Chemical bond; Tunnel effect; Ethylene; Molecular dynamics method; Molecular dynamics; Theoretical study; Electrode electrolyte interface; Review; Modeling; Lithium battery; Manganese oxides; Electronic structure; Electrolyte; Electrode reaction; Spinels; Electrochemical electrodes; Graphite; Numerical simulation; Lithium oxide; Ab initio calculations; Carbonates; Interface reaction; Electrochemical reaction; Interface
• ISSN: 1932-7447; 1932-7455
• DOI: 10.1021/jp308929a

We review recent ab initio molecular dynamics studies of electrode/electrolyte interfaces in lithium ion batteries. Our goals are to introduce experimentalists to simulation techniques applicable to models which are arguably most faithful to experimental conditions so far, and to emphasize to theorists that the inherently interdisciplinary nature of this subject requires bridging the gap between solid and liquid state perspectives. We consider liquid ethylene carbonate (EC) decomposition on lithium intercalated graphite, lithium metal, oxide-coated graphite, and spinel manganese oxide surfaces. These calculations are put in the context of more widely studied water–solid interfaces. Our main themes include kinetically controlled two-electron-induced reactions, the breaking of a previously much neglected chemical bond in EC, and electron tunneling. Future work on modeling batteries at atomic length scales requires capabilities beyond state-of-the-art, which emphasizes that applied battery research can and should drive fundamental science development.