Alignment of multi-wall carbon nanotubes by disentanglement in ultra-thin melt-drawn polymer films

Aligned multi-wall carbon nanotube (MWCNT)/polymer composite films were created in a one-step process. 5 wt% MWCNT/semi-crystalline polymer composite films of approximately 100nm thickness were obtained by melt-drawing. The matrix polymers were isotactic polypropylene (iPP), poly(1-butene) (PB-1) and high density polyethylene (HDPE). Transmission electron microscopy (TEM) investigations revealed an exceptionally high degree of local MWCNT alignment with an angular deviation of <10°<10° (HDPE) and <20°<20° (iPP and PB-1) parallel to the films’ drawing direction for a broad range of drawing velocities. For HDPE, the lamellar polymer-crystals at the interface between the MWCNT and the polymer film were identified as the nano-hybrid shish-kebab morphology by selected area electron diffraction. Based on the direct visualization of the MWCNT disentanglement process in the TEM, a polymer physics-based model for the unraveling of MWCNT entanglements, a source of aligned MWCNTs, is proposed that explains differences in MWCNT alignment encountered for different matrix polymers. The melt-drawing mediated MWCNT alignment provides both an innovative approach for the fabrication of applicable MWCNT containing films and a versatile tool for studying the interface in MWCNT/polymer composites.