Optimizing
the interactions between the matrix and reinforcement
components is key to attaining high-performance composite materials.
Yet, balancing the reinforcing–matrix phase interactions for
synthetic composites remains a great challenge. Here, a combined methodology
using molecular and atomic layer deposition (M/ALD) is demonstrated
for tailoring carbon nanotube (CNT) interfacial interactions, yielding
high-performance-reinforced polymer composites. CNT mats are used
as a model system to systematically study the molecular details as
they do not involve powder processing and other aspects which obscure
the understanding of molecular level effects. Noncovalent attachment
of the M/ALD layer at the interface allows good wetting of the CNTs,
provides an effective means for stress dissipation without compromising
the CNTs’ Csp2–Csp2 network which
remains intact, while introducing amine functionalities to facilitate
the cross-linking polymer matrix (epoxy). M/ALD-modified CNT mat–epoxy
composites showed an increase in the maximal tensile strength and
toughness of up to 32 and 247%, respectively. These findings may pave
the way to systematically develop high CNT loading composites as well
as other nano-reinforced composite systems showing both high strength
and toughness as well as numerous other desirable properties related
to nanomaterial composites in general.