Porous architectures for silicon/graphite (Si/Gr) composites
can
buffer the massive volume expansion of Si particles during electrochemical
cycling. However, the large surface area derived from the high porosity
leads to unavoidable side reactions at the electrode–electrolyte
interface, leading to the formation of thick resistive natural solid–electrolyte
interphase (SEI). Herein, a simple and scalable route is developed
for coating a polymeric artificial SEI (A-SEI) inside the porous architecture
for the Si/Gr composite via a facile incipient wetness impregnation
(IWI) method. Cross-sectional focused ion beam microscopic results
infer that the polymer coating is successful. Polymer coating for
the porous matrix as A-SEI induces sufficient porosity as well as
prevents excessive electrolyte penetration into the highly porous
matrix. Furthermore, it prevents the direct contact of active materials
with electrolytes, minimizing the parasitic reactions that form natural
SEIs. Consequently, the polymer coating obtained by IWI enables remarkable
enhancement in the long-cycle stability of the porous Si/Gr electrode,
in contrast to the nonimpregnated electrode displaying capacity roll-over
due to excessive SEI formation. Moreover, it is demonstrated that
the coating effectively prevents the formation of dendritic lithium
plating on the surface of the Si/Gr electrode, thereby enhancing the
safety of the battery.