Previous studies have demonstrated that chemical vapor
deposition
carbon coating on silicon (Si@C) can enhance the electrochemical performance
of lithium-ion batteries with Si-based anodes. However, the underlying
mechanisms contributing to this improvement have not been fully explored.
We address this knowledge gap by applying a suite of characterization
methods to evaluate Si@C anodes prepared by reducing acetylene on
ball-milled Si particles. Raman mapping measurements show that the
C coating (<5 nm thick) enables a homogeneous Si and carbon distribution
during the slurry casting process, thereby promoting Si utilization
during cycling. The coating’s microstructure and morphology
were evaluated using X-ray photoelectron spectroscopy (XPS), scanning
transmission electron microscopy, and neutron reflectivity experiments.
Electrochemical impedance spectroscopy measurements upon cycling indicate
that carbon coating also reduces the overall resistance as benchmarked
against bare Si anodes. Galvanostatic cycling in half-cell studies
revealed higher initial Coulombic efficiency and specific capacities
with increasing carbon coating time. However, solid electrolyte interphase
(SEI) investigations using XPS showed that the coated and uncoated
samples have very similar characteristics, suggesting that the SEI
may only play a minor role in enhancing the performance of Si@C. Full-cell
evaluation of the Si electrodes was consistent with half-cell results
relating to performance and SEI properties, further supporting the
conclusion that electronic and ionic percolation, enabled by effective
electrode manufacturing, are the dominant factors contributing to
the favorable performance of Si@C.