Publications Details
First-principles modeling of the initial stages of organic solvent decomposition on Li xMn 2O 4(100) surfaces
Density functional theory and ab initio molecular dynamics simulations are applied to investigate the initial steps of ethylene carbonate (EC) decomposition on spinel Li 0.6Mn 2O 4(100) surfaces. EC is a key component of the electrolyte used in lithium ion batteries. We predict a slightly exothermic EC bond-breaking event on this oxide facet, which facilitates subsequent EC oxidation and proton transfer to the oxide surface. Both the proton and the partially decomposed EC fragment weaken the Mn-O ionic bonding network. Implications for an interfacial film made of decomposed electrolyte on cathode surfaces, and Li xMn 2O 4 dissolution during power cycling, are discussed. © 2012 American Chemical Society.