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

137 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

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Encapsulation
Energy storage
Oxides
Nanocomposites
Permittivity
Metals
Nanoparticles
Dielectric losses
Leakage currents
Polypropylene oxides
Aluminum Oxide
Polyolefins
Zirconium
Propylene
Raman spectroscopy
Fillers
Differential scanning calorimetry
Atomic force microscopy
Volume fraction
Current density

ASJC Scopus subject areas

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

Cite this

In situ catalytic encapsulation of core-shell nanoparticles having variable shell thickness : Dielectric and energy storage properties of high-permittivity metal oxide nanocomposites. / Li, Zhong; Fredin, Lisa A.; Tewari, Pratyush; Dibenedetto, Sara A.; Lanagan, Michael T.; Ratner, Mark A; Marks, Tobin J.

In: Chemistry of Materials, Vol. 22, No. 18, 28.09.2010, p. 5154-5164.

Research output: Contribution to journalArticle

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