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

Abstract

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 lengthscales requires capabilities beyond state-of-the-art, which emphasizes that applied battery research can and should drive fundamental science development.

24 pages, 4 figures

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Cited by in corpus (9)

• Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes from First Principles and Classical Reactive Molecular Dynamics
• Modeling Electrochemical Decomposition of Fluoroethylene Carbonate on Silicon Anode Surfaces in Lithium Ion Batteries
• First Principles Modeling of Mn(II) Migration above and Dissolution from Li(x)Mn(2)O(4) (001) Surfaces
• Towards First Principles prediction of Voltage Dependences of Electrolyte/Electrolyte Interfacial Processes in Lithium Ion Batteries
• DFT Modelling of Explicit Solid-Solid Interfaces in Batteries: Methods and Challenges
• Insights into lithium manganese oxide-water interfaces using machine learning potentials
• Interface identification of the solid electrolyte interphase on graphite
• Enhancing ReaxFF for Molecular Dynamics Simulations of Lithium-Ion Batteries: An interactive reparameterization protocol
• Exponential Scaling of Water Exchange Rates with Ion Interaction Strength from the Perspective of Dynamic Facilitation Theory