Chirality-Dependent Mechanical Properties of Bundles and Thin Films Composed of Covalently Cross-Linked Carbon Nanotubes.

Abstract

The effect of nanotube chirality on the mechanical properties of materials composed of single-walled carbon nanotubes (CNTs) is poorly understood since the interfacial load transfer in such materials is strongly dependent on the intertube interaction and structure of the nanotube network. Here, a combined atomistic-mesoscopic study is performed to reveal the effect of CNT diameter on the deformation mechanisms and mechanical properties of CNT bundles and low-density CNT films with covalent cross-links (CLs). First, the pullout of the central nanotube from bundles composed of seven (5,5), (10,10), (20,20), (17,0), and (26,0) CNTs is studied in molecular dynamics simulations based on the ReaxFF force field. The simulations show that the shear modulus and strength increase with decreasing CNT diameter. The results of atomistic simulations are used to parametrize a mesoscopic model of CLs and to perform mesoscopic simulations of in-plane tension and compression of thin films composed of thousands of cross-linked CNTs. The mechanical properties of CNT films are found to be strongly dependent on CNT diameter. The film modulus increases as the CNT diameter increases, while the tensile strength decreases. The in-plane compression is characterized by collective bending of whole films and order-of-magnitude smaller compressive strengths. The films composed of (5,5) CNTs exhibit the ability for large-strain compression without irreversible changes in the material structure. The stretching rigidity of individual nanotubes and volumetric CL density are identified as the key factors that dominate the effect of CNT chirality on the mechanical properties of CNT films. The film modulus is affected by both CL density and stretching rigidity of CNTs, while the tensile strength is dominated by CL density. The obtained results suggest that the on-demand optimization of the mechanical properties of CNT films can be performed by tuning the nanotube chirality distribution.