Integrating carbon
nanotubes (CNTs) in carbon-fiber-reinforced-polymer (CFRP) composites
enhances structural and functional properties; however, it often involves
chemical functionalization or processes that lead to inhomogeneous
dispersion and nonuniform distribution of CNTs that impair the final
properties and hinder manufacturing scalability. Herein, we present
a novel and scalable processing technique to integrate pristine CNTs
(pCNTs) into CFRP composites without the need for chemical functionalization
or addition of surfactants. We use cellulose nanocrystals (CNCs) as
assisting nanomaterials to uniformly disperse and stabilize pCNTs
in water, and then we coat carbon fibers (CFs) with CNC-pCNT prior
to resin infusion. Two coating methods are used: simple immersion
(I-coating) and simultaneous immersion and sonication (IS-coating).
The surface chemistry of coated CFs reveals that I-coating provides
a higher quantity of polar oxygen groups in coated CFs containing
CNC-pCNT compared to IS-coating. We show that fabricating hybrid CFRPs
by incorporating 0.2 wt % CNC–0.2 wt % pCNT in CFRP composites
using this simple technique enhances the flexural strength by 33%
and the interlaminar shear strength (ILSS) by 35% compared to those
of neat CFRPs. Significantly, 0.2CNC-0.2pCNT-CFRPs show ∼25%
higher flexural strength and ILSS compared to the largest enhancement
in composites with individual functionalized CNTs (fCNTs) or CNCs,
demonstrating a synergistic effect of CNC-pCNT in enhancing properties.
Moreover, our results indicate that incorporating CNC-pCNT increases
the thermal stability of CFs compared to those of fCNTs. These are
specifically crucial in composites used in structural applications.
These results highlight that the introduced CNC-enabled processing
technique is a potential scalable path toward the fabrication of hybrid
composites that can enhance properties higher than individual CNTs
or CNCs, avoiding costly and/or time-inefficient functionalization
processes.