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Previous and current research on piezoresistivity of polymer composites filled with carbon nanostructures is reviewed. The review covers the use of the coupled electro‐mechanical response of these materials to self‐sense their strain and damage during mechanical loading. The mechanisms yielding changes in electrical resistance upon mechanical loading in polymer composites filled with carbon nanostructures are first discussed. Published knowledge is then summarized, starting with framework literature on carbon black and graphite and then moving to more recent research on carbon nanotubes, exfoliated graphite, and few‐layer graphene sheets. Piezoresistive studies of polymer nanocomposites with aligned carbon fillers are also reviewed. It is aimed that this review contributes in collecting, organizing, and summarizing the knowledge, foundations, and state of the art on the piezoresistive response of polymer composites filled with different carbon allotropes, providing new perspectives and advancing towards the fast development of smart self‐sensing carbon filled nanocomposites.

The dynamics of multiwall carbon nanotube (MWCNT) alignment inside viscous media using electric fields is investigated. Electrical current measurements were performed in situ during the application of an electric field to liquid solutions of deionized water or dissolved polymer containing MWCNTs. The variation of electrical current over time was associated to the dynamics of the MWCNT network formation. The influence of the electric field magnitude and frequency on the MWCNT network formation was studied. MWCNT migration towards the negative electrode was observed when a direct current electric field was applied, whereas formation of an aligned MWCNT network was achieved for an alternating current electric field. The increase of the electric field frequency promotes a faster formation of an aligned MWCNT network and thinner MWCNT bundles. A higher viscosity of the liquid medium yields slower MWCNT alignment evidenced by a slower change of electrical current through the viscous system. An analytical model based on the dielectrophoresis-induced torque, which considers the viscosity of the medium, is also proposed to explain the dynamics of MWCNT alignment. Furthermore, aligned MWCNT/polysulfone solid composites were fabricated and electrically characterized. The solid composites presented anisotropic electrical conductivity, which was more evident for low MWCNT concentrations (0.1-0.2 wt%).

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