Two-dimensional (2D) siloxene (Si6O3H6) has shown promise as a negative electrode material
for Li-ion
batteries due to its high gravimetric capacity and superior mechanical
properties under (de)lithiation compared to bulk Si. In this work,
we prepare purified siloxene nanosheets through the removal of bulk
Si contaminants, use ultrasonication to control the lateral size and
thickness of the nanosheets, and probe the effects of the resulting
morphology and purity on the electrochemistry. The thin siloxene nanosheets
formed after 4 h of ultrasonication deliver an average capacity of
810 mA h/g under a 1000 mA/g rate over 200 cycles with a capacity
retention of 76%. Interestingly, the purified siloxene shows lower
initial capacity but superior capacity retention over extended cycling.
The 2D morphology benefit is illustrated where the parent siloxene
nanosheet morphology and structure were largely maintained based on operando optoelectrochemistry, in situ Raman, ex situ scanning
electron microscopy, and ex situ transmission electron microscopy.
Furthermore, the purified siloxene-based electrode free from crystalline
Si impurity experiences the least expansion upon (de)lithiation as
visualized by cross-section electron microscopy of samples recovered
post-cycling.