First Principles Modeling of the Initial Stages of Organic Solvent Decomposition on Li(x)Mn(2)O(4) (100) Surfaces

Abstract

Density functional theory and ab initio molecular dynamics simulations are applied to investigate the initial steps of ethylene carbonate (EC) decomposition on spinel Li(0.6)Mn(2)O(4) (100) surfaces. EC is a key component of the electrolyte used in lithium ion batteries. We predict an 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 interfacial film made of decomposed electrolyte on cathode surfaces, and Li(x)Mn(2)O(4) dissolution during power cycling, are discussed.

29 pages preprint format, 7 figures

References in corpus (2)

• Using atomic layer deposition to hinder solvent decomposition in lithium ion batteries: first principles modeling and experimental studies
• Cobalt-Porphyrin Catalyzed Electrochemical Reduction of Carbon Dioxide in Water II: Mechanism from First Principles

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