Extreme volume changes and concomitant
mechanical instabilities
(viz., origin and proliferation of cracking) in Si-based anodes are
responsible for premature failure in lithium-ion batteries. Thus,
it is a crucial hurdle toward the development of high-performance
Si-based batteries, especially in the current scenario of electric
vehicles. Accordingly, this research demonstrates a significant improvement
in the mechanical stainability of Si-based anode material via in situ incorporation of carbide with a specific design,
thereby bestowing outstanding stability in the electrochemical performance.
At this juncture, we have established a bridge between nanomechanical
and electrochemical properties, investigated via nanoindentation and in-operando stress measurements during electrochemical cycling
for Si and in situ reinforced Si–SiC composite.
Enhancing the hardness (H) of Si–SiC composite
to almost twice as well as enhancing the hardness to effective Young’s
modulus (E*) ratio (H
3/E*2) of the same to almost thrice than
that of Si, helped resist the occurrence of plastic deformation and
cracking in significant terms. In-operando study
shows the typical stress flattening (cum, anisotropic behavior) in
the case of the unreinforced Si electrode, which is a manifestation
of plastic flow/cracking. By contrast, monotonous stress profiles
and absence of the signature of plastic flow/cracking are observed
for the Si–SiC electrode, which is an advantage for long cycle
life, as observed here. Overall, this kind of experimental study could
establish the nanomechanical to electrochemical tie-up, leading to
82% capacity retention over 650 cycles in a Li-ion full-cell along
with the Si–SiC composite anode. The “power cycle”
of the Si–SiC composite anode, with a variation of current
density from 0.5 to 6.0 A g–1, also reveals excellent
stability up to 2500 cycles.