In this study, a strategy for the fabrication of zirconia-polyimide (ZrO 2 -PI) nanohybrid films with high permittivity (high-k), thermal stability, and excellent mechanical properties has been developed. A colloidal suspension of ZrO 2 nanorods was prepared using the facile microwave-hydrothermal treatment approach. The ZrO 2 -PI nanohybrid film was fabricated by casting an aqueous solution containing water-soluble poly(amic acid) ammonium salt (PAS) and water-dispersible ZrO 2 nanorods followed by thermal imidization. Atomic force microscopy and scanning electron microscopy images indicated that the ZrO 2 nanorods were uniformly dispersed in the PI matrix. Because of the high permittivity of the ZrO 2 nanorods and good compatibility between polyimide and ZrO 2 as well as the nanosize of ZrO 2 , the permittivity increased to 5.1 as the ZrO 2 concentration reached 10% at 10 Hz, while the dielectric loss was as low as 0.05 at 10 Hz. The prepared ZrO 2 -PI nanohybrid films had excellent heat resistance with quite low coefficients of thermal expansion (CTE), as low as 16.3 ppm/K. The ZrO 2 -PI nanohybrid films have excellent thermal stability and good mechanical flexibility. Moreover, no distinct changes were observed for the PAS solution over a storage time of 3 months, after which the nanohybrid film could still be successfully synthesized by thermal imidization. In addition, the water uptake of the ZrO 2 -PI nanohybrid film was approximately 2.5% under 60% relative humidity. The high stability of the PAS precursor, good flexibility, enhanced permittivity, and low CTE behavior of the ZrO 2 -PI nanohybrid films could make this strategy attractive for the ecofriendly design of dielectric polymer nanohybrids as well as for the fabrication of nanohybrid films with potential applications in high charge-storage capacitors and organic field-effect transistors (OFETs) in the flexible electronics industry.
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