Ushirogata, K; Sodeyama, K; Futera, Z; Tateyama, Y; Okunoa, Y; (2015) Near-Shore Aggregation Mechanism of Electrolyte Decomposition Products to Explain Solid Electrolyte Interphase Formation. Journal of The Electrochemical Society , 162 (14) A2670-A2678. 10.1149/2.0301514jes.

Preview

Text 2015_JElchemSoc_162_Ushirogata.pdf - Published Version Download (857kB) | Preview

Abstract

To get insight of the formation mechanism of solid electrolyte interphase (SEI) film in Lithium-ion battery (LIB), we examine a probable scenario, referred to as “surface growth mechanism,” for electrolyte involving ethylene carbonate (EC) solvent and vinylene carbonate (VC) additive by using density functional theory (DFT). We first extracted stable SEI film components (SFCs) for the EC/VC electrolyte and constructed probable SFC aggregates via DFT molecular dynamics. We then examined their solubility in the EC solution, their adhesion to a model graphite electrode, and the electronic properties. The results showed that the SFC aggregates are characterized by “unstable adhesion” to the graphite surface and “high electronic insulation” against the EC solution. These characteristics preclude explaining SEI growth up to a typical thickness of several tens of nanometers based on the surface growth mechanism. With the present results, we propose “near-shore aggregation” mechanism, where the SFCs formed at the electrode surface desorb into the near-shore region and form aggregates. The SFC aggregates coalesce and come into contact with the electrode to complete the SEI formation. The present model provides a novel perspective for the long-standing problem of SEI formation.

Download activity - last month

Export as XMLJSONCSV

Download activity - last 12 months

Export as XMLJSONCSV

Downloads by country - last 12 months

Export as CSVJSONXML

Archive Staff Only

View Item