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Carbon nanotube/glass fiber hierarchical composite structures have been produced using an electrophoretic deposition (EPD) approach for integrating the carbon nanotubes (CNTs) into unidirectional E-glass fabric, followed by infusion of an epoxy polymer matrix. The resulting composites show a hierarchical structure, where the structural glass fibers, which have diameters in micrometer range, are coated with CNTs having diameters around 10-20 nm. The stable aqueous dispersions of CNTs were produced using a novel ozonolysis and ultrasonication technique that results in dispersion and functionalization in a single step. Ozone-oxidized CNTs were then chemically reacted with a polyethyleneimine (PEI) dendrimer to enable cathodic EPD and promote adhesion between the CNTs and the glass-fiber substrate. Deposition onto the fabric was accomplished by placing the fabric in front of the cathode and applying a direct current (DC) field. Microscopic characterization shows the integration of CNTs throughout the thickness of the glass fabric, where individual fibers are coated with CNTs and a thin film of CNTs also forms on the fabric surfaces. Within the composite, networks of CNTs span between adjacent fibers, and the resulting composites exhibit good electrical conductivity and considerable increases in the interlaminar shear strength, relative to fiber composites without integrated CNTs. Mechanical, chemical and morphological characterization of the coated fiber surfaces reveal interface/interphase modification resulting from the coating is responsible for the improved mechanical and electrical properties. The CNT-coated glass-fiber laminates also exhibited clear changes in electrical resistance as a function of applied shear strain and enables self-sensing of the transition between elastic and plastic load regions.

The electrophoretic deposition (EPD) method was used to deposit polyethylenimine (PEI) functionalized multiwall carbon nanotube (CNT) films onto the surface of individual S-2 glass fibers. By varying the processing parameters of EPD following Hamaker's equation, the thickness of the CNT film was controlled over a wide range from 200 nm to 2 μm. The films exhibited low electrical resistance, providing evidence of coating uniformity and consolidation. The effect of the CNT coating on fiber matrix interfacial properties was investigated through microdroplet experiments. Changes in interfacial properties due to application of CNT coatings onto the fiber surface with and without a CNT-modified matrix were studied. A glass fiber with a 2 μm thick CNT coating and the unmodified epoxy matrix showed the highest increase (58%) in interfacial shear strength (IFSS) compared to the baseline. The increase in the IFSS was proportional to CNT film thickness. Failure analysis of the microdroplet specimens indicated higher IFSS was related to fracture morphologies with higher levels of surface roughness. EPD enables the thickness of the CNT coating to be adjusted, facilitating control of fiber/matrix interfacial resistivity. The electrical sensitivity provides the opportunity to fabricate a new class of sizing with tailored interfacial properties and the ability to detect damage initiation.

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