Abstract

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.

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