Feigned death induced by partial delithiation in silicon composite electrodes

Abstract

This paper discovers and reveals a phenomenon of feigned death induced by partial delithiation in silicon composite electrodes. Unexpected extremely rapid capacity fading occurs in the initial dozens of the cycles with low upper cut-off voltages. By looking into the irreversibility, the crack, the elemental analysis and the thickness/weight of the electrode, it suggests that the rapid capacity fading is not induced by degradation. Additionally, by providing a reboot with full delithiation, the capacity can be recovered completely, which confirms the integrity of the electrode. This novel type of capacity fading is named by “feigned death” to distinguish it from the “true death” caused by degradation. It is further confirmed that the feigned death is caused by the asymmetric phase transformation between crystalline and amorphous phases in silicon electrodes. When the depth of lithiation is high enough to generate the c-Li3.75Si phase but the depth of delithiation is too low to eliminate the generated crystalline phase, the feigned death is triggered. The findings of this work provide an in-depth understanding of the electrochemical performance of Si-based electrodes.