Failure mechanisms in lithium silicon batteries

Abstract

Lithium silicon (Li-Si) batteries offer more than ten times the theoretical specific capacity compared to current lithium ion battery technologies, by using a silicon anode. In practice however, the cycle life of Li-Si batteries is very limited. The large volume change of the silicon anode is known to be the main reason for this. Research on the volume changes during varying cell cycles and voltages is presented in this thesis and an experimental set up for a quasi in situ study of the SEI layer is suggested. Cycling tests with an amorphous silicon thin film of 220 nm deposited using magnetron sputtering on a copper foil current collector confirmed that the major cause of capacity loss is swelling of the silicon during lithiation, causing the silicon to detach from the current collector and resulting in significant capacity loss. Increasing the lower cut off voltage from 0 V to 0.2 V resulted in a slight improvement of cycle life. Silicon detachment also decreased as determined by SEM images. EFTEM and EDX mapping showed a clear split between a partially lithiated silicon layer on the surface and a pure silicon layer on the current collector side. It can be concluded that discharging Li-Si batteries to 0.2 V instead of 0 V is a promising method to reduce the swelling of silicon during lithiation.