Nanoparticle, Size, Shape, and Interfacial Effects on Leakage Current Density, Permittivity, and Breakdown Strength of Metal Oxide-Polyolefin Nanocomposites: Experiment and Theory

Neng Guo, Sara A. DiBenedetto, Pratyush Tewari, Michael T. Lanagan, Mark A Ratner, Tobin J Marks

Research output: Contribution to journalArticle

181 Citations (Scopus)

Abstract

A series of 0-3 metal oxide-polyolefin nanocomposites are synthesized via in situ olefin polymerization, using the following single-site metallocene catalysts: C2-symmetric dichloro[rac-ethylenebisindenyl]-zirconium(IV),Me 2Si( tBuN)(η 5-C 5Me 4)TiCl 2, and(η 5-C 5Me 5)TiCl 3 immobilized onmethylaluminoxane (MAO)-treated BaTiO 3, ZrO 2, 3-mol %-yttria-stabilized zirconia, 8-mol%-yttria-stabilized zirconia, sphere-shaped TiO2 nanoparticles, and rod-shaped TiO 2 nanoparticles. The resulting compositematerials are structurally characterized via X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), 13C nuclear magnetic resonance (NMR) spectroscopy, and differential scanning calorimetry (DSC). TEM analysis shows that the nanoparticles are well-dispersed in the polymer matrix, with each individual nanoparticle surrounded by polymer. Electrical measurements reveal that most of these nanocomposites have leakage current densities of ∼10 -6-10 -8 A/cm 2; relative permittivities increase as the nanoparticle volume fraction increases, withmeasured values as high as 6.1. At the same volume fraction, rod-shaped TiO 2 nanoparticle-isotactic polypropylene nanocomposites exhibit significantly greater permittivities than the corresponding sphere-shaped TiO 2 nanoparticleisotactic polypropylene nanocomposites. Effective medium theories fail to give a quantitative description of the capacitance behavior, but do aid substantially in interpreting the trends qualitatively. The energy storage densities of these nanocomposites are estimated to be as high as 9.4 J/cm 3.

Original languageEnglish
Pages (from-to)1567-1578
Number of pages12
JournalChemistry of Materials
Volume22
Issue number4
DOIs
Publication statusPublished - Feb 23 2010

Fingerprint

Polyolefins
Leakage currents
Oxides
Nanocomposites
Permittivity
Current density
Metals
Nanoparticles
Polypropylenes
Experiments
Yttria stabilized zirconia
Volume fraction
Transmission electron microscopy
Monoamine Oxidase
Alkenes
Polymer matrix
Zirconium
Energy storage
Nuclear magnetic resonance spectroscopy
Olefins

ASJC Scopus subject areas

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

Cite this

Nanoparticle, Size, Shape, and Interfacial Effects on Leakage Current Density, Permittivity, and Breakdown Strength of Metal Oxide-Polyolefin Nanocomposites : Experiment and Theory. / Guo, Neng; DiBenedetto, Sara A.; Tewari, Pratyush; Lanagan, Michael T.; Ratner, Mark A; Marks, Tobin J.

In: Chemistry of Materials, Vol. 22, No. 4, 23.02.2010, p. 1567-1578.

Research output: Contribution to journalArticle

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abstract = "A series of 0-3 metal oxide-polyolefin nanocomposites are synthesized via in situ olefin polymerization, using the following single-site metallocene catalysts: C2-symmetric dichloro[rac-ethylenebisindenyl]-zirconium(IV),Me 2Si( tBuN)(η 5-C 5Me 4)TiCl 2, and(η 5-C 5Me 5)TiCl 3 immobilized onmethylaluminoxane (MAO)-treated BaTiO 3, ZrO 2, 3-mol {\%}-yttria-stabilized zirconia, 8-mol{\%}-yttria-stabilized zirconia, sphere-shaped TiO2 nanoparticles, and rod-shaped TiO 2 nanoparticles. The resulting compositematerials are structurally characterized via X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), 13C nuclear magnetic resonance (NMR) spectroscopy, and differential scanning calorimetry (DSC). TEM analysis shows that the nanoparticles are well-dispersed in the polymer matrix, with each individual nanoparticle surrounded by polymer. Electrical measurements reveal that most of these nanocomposites have leakage current densities of ∼10 -6-10 -8 A/cm 2; relative permittivities increase as the nanoparticle volume fraction increases, withmeasured values as high as 6.1. At the same volume fraction, rod-shaped TiO 2 nanoparticle-isotactic polypropylene nanocomposites exhibit significantly greater permittivities than the corresponding sphere-shaped TiO 2 nanoparticleisotactic polypropylene nanocomposites. Effective medium theories fail to give a quantitative description of the capacitance behavior, but do aid substantially in interpreting the trends qualitatively. The energy storage densities of these nanocomposites are estimated to be as high as 9.4 J/cm 3.",
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