Electrode-electrolyte interface molecular dynamics simulations

Xing, L. D. Vatamanu, J. Borodin, O. Smith, G. D. Bedrov, D., Electrode/Electrolyte Interface in Sulfolane-Based Electrolytes for Li Ion Batteries A Molecular Dynamics Simulation Study. J. Phys. Chem. C 2012,116, 23871-23881. 

The primary molecular modeling methods that have been extensively applied to lithium battery electrolytes and electrode/electrolyte interfaces are molecular orbital calculations and molecular dynamics simulations. The former involves ab initio and density functional methods and will be referred to quanmm chemistry or QC... 

Molecular Dynamics Simulations of Electrode/Electrolyte Interfaces... 

In the next section a brief layout of simulation methods will be given. Then, some basic properties of the models used in computer simulations of electrochemical interfaces on the molecular level will be discussed. In the following three large sections, the vast body of simulation results will be reviewed structure and dynamics of the water/metal interface, structure and dynamics of the electrolyte solution/metal interface, and microscopic models for electrode reactions will be analyzed on the basis of examples taken mostly from my own work. A brief account of work on the adsorption of organic molecules at interfaces and of liquid/liquid interfaces complements the material. In the final section, a brief summary together with perspectives on future work will be given. 

Abstract Recent advances in molecular modeling provide significant insight into electrolyte electrochemical and transport properties. The first part of the chapter discusses applications of quantum chemistry methods to determine electrolyte oxidative stability and oxidation-induced decomposition reactions. A link between the oxidation stability of model electrolyte clusters and the kinetics of oxidation reactions is established and compared with the results of linear sweep voltammetry measurements. The second part of the chapter focuses on applying molecular dynamics (MD) simulations and density functional theory to predict the structural and transport properties of liquid electrolytes and solid elecfiolyte interphase (SEI) model compounds the free energy profiles for Uthium desolvation from electrolytes and the behavior of electrolytes at charged electrodes and the electrolyte-SEl interface. 

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