Date of Award

12-2013

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Legacy Department

Chemical Engineering

Advisor

Ogale, Amod A

Committee Member

Hubing, Todd H

Committee Member

Hirt, Douglas E

Committee Member

Kitchens, Christopher L

Abstract

Conductive polymer composites have become alternative materials for providing electromagnetic and electrostatic shielding where metals are not suitable. In this study, the effect of crystallinity, morphology, concentration and orientation of carbon nanomodifiers on shielding provided by their polyethylene-based composites has been investigated relative to their transport properties.

First, the electrical properties and EM SE of composites consisting of heat-treated carbon nanofibers (Pyrograf® -III PR-19 CNF) in a linear low density polyethylene (LLDPE) matrix were assessed. Heat treatment (HT) of CNF at 2500°C significantly improved their graphitic crystallinity and intrinsic transport properties, thereby increasing the EM SE of the nanocomposites. Although the strain-to-failure was about one-third that of pure LLDPE, the absolute value of 180±98% indicates a significant retention of ductility.

Second, the influence of the morphology of carbon modifiers on the electrical, thermal and mechanical properties of their composites was investigated. Four heat-treated carbon modifiers were investigated: PR-19 HT carbon nanofibers, multi-walled carbon nanotubes (MWNT HT), helical multi-walled carbon nanotubes (HCNT HT), and pitch-based P-55 carbon fibers (CF). MWHT HT, with the highest aspect ratio, led to the largest composite electrical and thermal conductivities (34 S/m, 1 W/m.K) and EM SE (~24 dB). In contrast, HCNT HT, due to their coiled shape and low aspect ratio, led to a non-percolating microstructure in the composites, which produced poor EM SE (dB). Nonetheless, HCNT HT composites displayed the highest ductility (~250%) and flexibility, which is probably owed to the matrix-modifier mechanical bonding (interlocking) provided by the helical morphology.

Using the carbon modifiers that previously led to the best EM SE (i.e., PR-19 HT and MWNT HT), the influence of composite electrical properties on the plane-wave EM SE in the VHF-UHF bands was studied further. Both graphitic nanomodifiers were dispersed in LLDPE matrix to produce a nominally random in-plane modifier orientation. For a concentration of 10 vol% nanomodifiers, EM SE values of 22 dB and 24 dB were obtained for PR-19 HT and MWNT HT nanocomposites (2.5-mm thick), respectively. At a high concentration of 40 vol%, EM SE values as high as 68 dB and 55 dB were respectively attained. Because such nanocomposites possess only moderate electrical conductivity, a model for generally-lossy materials was used to predict the plane-wave EM SE and its components. Based on the material properties of the nanocomposites, the predicted values of EM SE were found to be consistent with the experimental values.

Finally, the electrical conductivity and EM SE of nanocomposites that contained 10 vol% of oriented graphitic nanomodifiers (PR-19 HT and MWNT HT) in LLDPE are reported. Micro-filament spinning was used to generate flow-induced orientation of the carbon nanomodifiers. Consequently, the conductivity of the resulting nanocomposites exhibited anisotropy. Thus, the in-plane conductivity in the longitudinal direction (PR-19 HT comp.: ~0.02 S/m; MWNT HT comp.: ~3 S/m) was at least an order of magnitude higher than that along the transverse direction. As measured with a rectangular waveguide (WR510, 1.45-2.2 GHz), the PR-19 HT and MWNT HT oriented nanocomposites (1-mm thick) displayed EM SE values of 0.7±0.4 dB and 3.0±0.8 dB, respectively, when the nanomodifiers were transversely oriented with the polarized electric field. In contrast, when the orientation of the nanomodifiers was parallel with the field, values of 3.2±1.0 dB and 9.0±1.0 dB were obtained, respectively. Therefore, as a result of this anisotropy, as analyzed by polarized electromagnetic waves, the composites displayed anisotropic shielding. (Abstract shortened by UMI.)

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