Electrokinetics of scalable, electric-field-assisted fabrication of vertically aligned carbon-nanotube/polymer composites

Composite thin films incorporating vertically aligned carbon nanotubes (VACNTs) offer promise for a variety of applications where the vertical alignment of the CNTs is critical to meet performance requirements, e.g., highly permeable membranes, thermal interfaces, dry adhesives, and films with anisotropic electrical conductivity. However, current VACNT fabrication techniques are complex and difficult to scale up. Here, we describe a solution-based, electric-field-assisted approach as a cost-effective and scalable method to produce large-area VACNT composites. Multiwall-carbon nanotubes are dispersed in a polymeric matrix, aligned with an alternating-current (AC) electric field, and electrophoretically concentrated to one side of the thin film with a direct-current (DC) component to the electric field. This approach enables the fabrication of highly concentrated, individually aligned nanotube composites from suspensions of very dilute (ϕ=4×10−4) volume fraction. We experimentally investigate the basic electrokinetics of nanotube alignment under AC electric fields, and show that simple models can adequately predict the rate and degree of nanotube alignment using classical expressions for the induced dipole moment, hydrodynamic drag, and the effects of Brownian motion. The composite AC + DC field also introduces complex fluid motion associated with AC electro-osmosis and the electrochemistry of the fluid/electrode interface. We experimentally probe the electric-field parameters behind these electrokinetic phenomena, and demonstrate, with suitable choices of processing parameters, the ability to scalably produce large-area composites containing VACNTs at number densities up to 1010 nanotubes/cm2. This VACNT number density exceeds that of previous electric-field-fabricated composites by an order of magnitude, and the surface-area coverage of the 40 nm VACNTs is comparable to that of chemical-vapor-deposition-grown arrays of smaller-diameter nanotubes.