Great
efforts have been devoted to the development of high-energy-density
lithium-ion batteries (LIBs) to meet the requirements of emerging
technologies such as electric cars, large-scale energy storage, and
portable electronic devices. To this end, silicon-based electrodes
have been increasingly regarded as promising electrode materials by
virtue of their high theoretical capacity, low costs, environmental
friendliness, and high natural abundance. It has been noted that during
repeated cycling, severe challenges such as huge volume change remain
to be solved prior to practical application, which boosts the development
of advanced cross-linked binders via chemical bonds (CBCBs) beyond
traditional PVDF binder. This is because CBCBs can effectively fix
the electrode particles, inhibit the volume expansion of Si particles,
and stabilize the solid electrolyte interface and thus can enable
good cycling stability of silicon anode-based batteries. In light
of these merits, CBCBs hence arouse much attention from both industry
and academia. In this review, we present chemical/mechanical characteristics
of CBCBs and systematically discuss the recent advancements of cross-linked
binders via chemical bonding for silicon-based electrodes. Focus is
placed on the cross-linking chemistries, construction methods and
structure–performance relationships of CBCBs. Finally, the
future development and performance optimization of CBCBs are proposed.
This discussion will provide good insight into the structural design
of CBCBs for silicon-based electrodes.