Theoretical study of the reductive decomposition of ethylene sulfite: a film-forming electrolyte additive in lithium ion batteries.
The role of ethylene sulfite (ES) as an electrolyte additive for lithium ion batteries is explained by investigating the one- and two-electron reductive decomposition of ES and (ES)Li(+)(PC)(n) (n = 0-2), both in vacuum and solvent, with the aid of high-level density functional theory calculations. The open-chain radical, which is formed as a result of reduction of ES in solvent without first being coordinated with Li(+), is further stabilized by a dissolved lithium ion. The resulting more stable intermediate releases a somewhat large amount of energy, which is utilized in the formation of a subsequent radical anion. On the basis of the study on the reductive decomposition of ES, (ES)Li(+)(PC), and (ES)Li(+)(PC)(2), the major products that are responsible for the formation of a protective solid electrolyte interphase film are Li(2)SO(3), (CH(2)OSO(2)Li)(2), CH(3)CH(OSO(2)Li)CH(2)OCO(2)Li, and ROSO(2)Li.
Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei, 106, Taiwan, ROC.
Ermias Girma
EG
Leggesse
Jyh-Chiang
JC
Jiang