A study of evolution of residual stress in single crystal silicon electrode using Raman spectroscopy

Abstract

Silicon is a promising anode material for lithium ion batteries. However, lithiation of silicon generates stress that is known to be the primary reason for the failure of the anode. This study explored the existence of residual stress in single crystalline silicon electrodes after full de-lithiation, i.e., under no mechanical or electrical load. The magnitude of residual stress and its evolution with the number of lithiation-delithiation cycles is measured by Raman spectroscopy and a simple mechanics based approach. It is shown that the residual stress is tensile in nature and increased from 69 ± 11 MPa after the 1st cycle to ∼291 ± 56 MPa after 50 cycles of lithiation and de-lithiation. Concurrently, microstructural studies were performed to demonstrate the consequence of the evolution of residual stress on failure by the fracture of the silicon anode. These results provide understanding on the progressive failure mechanism of single crystalline-based silicon electrodes upon lithiation-delithiation.