The reductive mechanism of ethylene sulfite as solid electrolyte interphase film-forming additive for lithium ion battery

The reduction mechanism of ethylene sulfite (ES) in propylene carbonate (PC) based electrolyte is investigated using density functional theory in gas phase. Based on the electron affinity energy and lowest unoccupied molecular orbital (LUMO) energy, it can be known that free ES is reduced most easily compared with ES-Li(+) and ES-Li(+)-PC, generating SO(2) and propanal. However, the binding energy of ES-Li(+) and ES-Li(+)-PC is quite negative, indicating that both of them are more possible in electrolyte solution than the free ES. The reductive decomposition products of ES-Li(+) and ES-Li(+)-PC are OSO(2)Li, OSO(2)Li-R and ethylene. OSO(2)Li and OSO(2)Li-R are the main compositions of the solid electrolyte interphase film on the anode of lithium ion battery, which inhibits the reductive decomposition of PC. These calculations provide a detailed explanation on the experimental phenomena. (C) 2010 Elsevier B.V. All rights reserved.