Ever-increasing
electrification scenarios call for high energy
density (U
e) polymer nanodielectric films
beyond the commercial benchmark biaxially oriented polypropylene.
Ferroelectric polymers of intrinsic high dielectric constant εr, if integrated with improved breakdown strength (E
b) and dielectric loss from nanofillers, would
be a promising paradigm for high-U
e polymer
nanodielectrics. Yet, this expectation is still in its infancy because
of the great challenge of increasing the E
b and needs introduction of new approaches. Here, fluorographene (FG),
as a young halogen derivative of graphene, is employed as an emerging
nanofiller to develop high-E
b polymer
nanodielectrics. A dramatically enhanced E
b, which is 39.4% higher than
that of a neat polymer film from casting, is achieved in a composite
film along with a reduced dielectric loss by incorporating only 0.2
wt % FG with in-plane orientation from electrospinning. The origin
of such a high E
b-reinforcing effect of
FG is traced by both experimental characterizations and phase-field
simulation. It is found that the in-plane oriented FG of appropriate
loading level would induce both the favorable low crystallinity of
the polymer matrix and the FG–polymer interface with deep traps
and less defects. This, together with the high out-of-plane insulation
of FG from a high fluorine/carbon ratio, regulates the charge behaviors
and breakdown paths and thus significantly enhances the voltage endurance
of composite films. The results demonstrate the remarkable E
b-reinforcing effect of emerging FG fillers
in polymer nanodielectrics and offer a strategy toward high-E
b/high-U
e flexible
dielectric capacitors.