The development of high-power-density
energy storage devices and
systems calls for high-dielectric-constant (high-k) polymer films with low dielectric loss. Aromatic polythiourea attracts
many interests because of its low dielectric loss and high beakdown
strength, whereas the high brittleness significantly limits its application
as dielectric films. In this report, flexible high-k films were successfully fabricated by cross-linking aromatic thiourea
oligomers with allyl glycidyl ether grafted poly(methylhydrosiloxane)
(PMHS). Siloxane segments of PMHS improve the flexibility of the cross-linked
dielectric films, and the grafted glycidyl ether side groups of PMHS
provide highly polarizable building blocks. Because of the high dipole
moment (4.89 D), aromatic thiourea endows the dielectric films with
a high dielectric constant. Microphase separation morphology was found
within the film, and the self-assembly into layered lamellae contributed
to the scatter of high-energy-charge carriers. As a result, the dielectric
films exhibit reduced dielectric loss tangent and suppressed leakage
current density with a high dielectric constant of above 6, a promissing
energy density of 3.15 J/cm3 and a high efficiency of above
87% under an electric field of 350 MV/m.