Mechanical Damage of Surface Films and Failure of Nano-Sized Silicon Electrodes in Lithium Ion Batteries

Autor: Hosang Park, Jae Gil Lee, Eun Kyung Kim, Jongjung Kim, Seung M. Oh, Hyun-seung Kim, Jeong Beom Lee, Dong Sub Jung, Ji Heon Ryu
Rok vydání: 2016
Předmět:
Zdroj: Journal of The Electrochemical Society. 164:A6103-A6109
ISSN: 1945-7111
0013-4651
DOI: 10.1149/2.0141701jes
Popis: This work demonstrates that the mechanical damage of surface passivation films plays an underlying role in the failure of nano-sized Si electrodes in lithium-ion batteries. The surface film derived from the standard electrolyte (1.3 M LiPF6 dissolved in ethylene carbonate/diethyl carbonate) during the first lithiation step is damaged by the mechanical stress caused by the volume contraction of Si particles during the subsequent de-lithiation period. The electrolyte decomposes on the newly exposed Si surface and film deposition occurs, which is then mechanically damaged again owing to volume change of the Si particles. Such film deposition/damage cycles are repeated until the mechanical stress becomes insignificant as a result of capacity decay. Continued electrolyte decomposition, which prevails in the early cycling period, produces electronically insulating films located between Si particles, which cause Li trapping within the Si matrix. Li trapping is found to be responsible for the rapid decrease in capacity and Coulombic efficiency in the intermediate period of cycling. When fluoroethylene carbonate (FEC) is added to the electrolyte, a surface film that is robust against mechanical stress is produced. As a result, the FEC-derived surface film maintains its passivating ability and suppresses the irreversible reactions, resulting in a better cycling performance.
Databáze: OpenAIRE