To achieve multifunctional properties using nanocomposites,
selectively
locating nanofillers in specific areas by tailoring a mixture of two
immiscible polymers has been widely investigated. Forming a phase-separated
structure from entirely miscible molecules is rarely reported, and
the related mechanisms to govern the formation of assemblies from
molecules have not been fully resolved. In this work, a novel method
and the underlying mechanism to fabricate self-assembling, bicontinuous,
biphasic structures with localized domains made up of amine-functionalized
graphene nanoplatelets are presented, involving the tailoring of compositions
in a liquid processable multicomponent epoxy blend. Kinetics studies
were carried out to investigate the differences in reactivity of various
epoxy-hardener pairs. Molecular dynamics simulations and in
situ optical photothermal infrared spectroscopy measurements
revealed the trajectories of different components during the early
stages of polymerization, supporting the migration (phase behavior)
of each component during the curing process. Confirmed by the phase
structure and the correlated chemical maps down to the submicrometer
level, it is believed that the bicontinuous phase separation is driven
by the change of the miscibility between various building blocks forming
during polymerization, leading to the formation of nanofiller domains.
The proposed morphology evolution mechanism is based on combining
solubility parameter calculations with kinetics studies, and preliminary
experiments are performed to validate the applicability of the mechanism
of selectively locating nanofillers in the phase-separated structure.
This provides a simple yet sophisticated engineering model and a roadmap
to a mechanism for fabricating phase-separated structures with nanofiller
domains in nanocomposite films.