Metal-polymer dielectric composites show promising potential as embedded capacitors, whereas it remains a great challenge to achieve a high dielectric constant (εr) and low dielectric loss (tan δ) simultaneously. This work demonstrates a strategy for overcoming this challenge. Al nanoparticles with self-passivated ultrathin Al2O3 shells are compacted under the uniaxial pressure (P), and Al-epoxy composites are prepared by curing the liquid epoxy monomer that infiltrates into Al compacts. The contacting regions between adjacent Al nanoparticles are flattened and enlarged during the compacting process, so that the ultrathin Al2O3 parallel-plate microcapacitors are constructed by the insulating Al2O3 shells and conductive Al cores. The composite with P of 100 MPa and Al volume fraction (υAl) of 53.7% exhibits the εr of 189 at 10 kHz, which is much higher than the εr (48-102) of 0-3 type Al-polymer composites with similar υAl and even higher than the highest εr (160) reported in the Al-polymer composite with υAl > 80%. Furthermore, the present composites show low tan δ (<0.03) and good frequency and temperature stability of εr. The finite element simulation proves that the construction and enlargement of ultrathin Al2O3 parallel-plate microcapacitors dramatically increase the electric energy stored in Al2O3 and therefore greatly improve the εr.
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