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.

Thermal Stability of TiN Coated Cubic Boron Nitride Powder

“…However, the starting powder has also a slight shift compared to the theoretical band positions. It probably has its origin in impurities [ 41 ] or/and residual stresses [ 42 ].…”

“…However, the starting powder has also a slight shift compared to the theoretical band positions. It probably has its origin in impurities [41] or/and residual stresses [42]. However, Figure 10c,d shows that the TiN phase tempered under a nitrogen atmosphere also undergoes some recrystallization (compare Figure 3e).…”

Electroanalytical methods and their hyphenated techniques for novel ion battery anode research

“…One year later, Jana and co-workers studied the evolution of the stress generated in a single c-Si during lithiation which was the main cause of failure and fracture of these NIBAMs. 145 They demonstrated that in situ Raman was an ideal tool to understand the progressive failure mechanism of single c-Si anodes. Whilst Cabo-Fernandez and co-workers used Raman to investigate the (de)lithiation mechanism on carbon-coated ZnFe2O4 (ZFO) anode 146 which is a TMO-based NIBAM type.…”

Morphological evolution of a single crystal silicon battery electrode during lithiation and delithiation: An operando phase-contrast imaging study

“…Up to now, no consensus about the aging mechanisms has been achieved yet. In contrast to the enormous work on particle-based anodes, much less research was done using single crystalline silicon electrodes, although it is a well-defined model electrode [28][29][30][31][32][33][34] . Single-crystal silicon allows us to study the lithiation process in a system without any binder or conductive agent.…”

“…Operando neutron and X-ray reflectometry reveal the depth-dependent lithium concentration over several cycles, but no fractures were observed due to experimental limitations [32][33][34] . The mechanical stress within the (100) silicon was determined by Chon et al depending on the cell voltage 29 , whereas Jana et al elucidated the cycle-dependent change of the residual stress within the (100) Si-crystal 28 . An ex-situ electron microscopy study revealed cracking of (100) silicon after several cycles 30 , whereas the crack propagation depends on the crystal orientation 31,35 .…”