In situ catalytic encapsulation of core-shell nanoparticles having variable shell thickness: Dielectric and energy storage properties of high-permittivity metal oxide nanocomposites

Zhong Li, Lisa A. Fredin, Pratyush Tewari, Sara A. Dibenedetto, Michael T. Lanagan, Mark A. Ratner, Tobin J. Marks

Research output: Contribution to journalArticle

144 Citations (Scopus)

Abstract

Aluminum oxide encapsulated high-permittivity (-) BaTiO3 and ZrO2 core-shell nanoparticles having variable Al2O 3 shell thicknesses were prepared via a layer-by-layer methylaluminoxane coating process. Subsequent chemisorptive activation of the single-site metallocene catalyst [rac-ethylenebisindenyl]zirconium dichloride (EBIZrCl2) on these Al2O3-encapsulated nanoparticles, followed by propylene addition, affords 0-3 metal oxide-isotactic polypropylene nanocomposites. Nanocomposite microstructure is analyzed by X-ray diffraction, transmission electron microscopy, scanning electron microscopy, differential scanning calorimetry, atomic force microscopy, and Raman spectroscopy. The in situ polymerization process yields homogeneously dispersed nanoparticles in a polyolefin matrix. Electrical measurements indicate that as the concentration of the filler nanoparticles increases, the effective permittivity of the nanocomposites increases, affording - values as high as 6.2. The effective permittivites of such composites can be predicted by the Maxwell-Garnett formalism using the effective medium theory for volume fractions (νf) of nanoparticles below 0.06. The nanocomposites have leakage current densities of ∼10-7-10-9 A/cm2 at an electric field of 105 V/cm, and very low dielectric loss in the frequency range 100 Hz-1 MHz. Increasing the Al2O3 shell thickness dramatically suppresses the leakage current and high field dielectric loss in these nanocomposites.

Original languageEnglish
Pages (from-to)5154-5164
Number of pages11
JournalChemistry of Materials
Volume22
Issue number18
DOIs
Publication statusPublished - Sep 28 2010

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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