Production of carbon nanotube reinforced nanoprepregs and their characterization

Epoxy based thermoset prepregs has been dominated materials market particularly in the automotive and aerospace applications. However, thermoplastic polymers recently have drawn attention with their potential to overcome challenges such as long cure cycles, poor fracture toughness, low viscosities, limited shelf lives and non-recyclability of thermosets. Thermoplastic resins have offered several advantages including recyclability, high impact resistance, and high thermal stability. Reinforcement strategies in laminated composites included both matrix and interface toughening. For matrix toughening, dispersion of additives into the matrix has been the most preferred method. One of the disadvantages of this method is stemming from non-proper dispersion of nanomaterials in the matrix. Moreover, the increase in polymer viscosity associated to nanomaterials reduced polymer processability. Interface toughening in laminated composites could be in the form of film, particle, and nanofibers to hinder crack propagation and improve better load transfer between each plies. With the use of interface elements in thermoplastic laminated composites, the superior properties could be enhanced and transferred to overall composites. Carbon nanotubes (CNTs) are hollow structures in which graphite layers are placed in cylinder forms. The superior properties of CNTs is dependent on CNTs physical properties, chirality, and the number of walls. In the case of interlaminar toughening CNTs could be placed through different routes such as buckypaper interleaving, CNTs grown on fibers. In most of bucky paper applications, CNTs were dissolved in an appropriate solvent. However, the use of any solvents would significantly form low-volume fraction CNTs structures, and also not are not permitted in aerospace applications. In order to overcome these challenges, new methods have been studied, which embraced the synthesis of CNTs structures on fiber substrates. By direct growth of CNTs onto fiber surface enabled the integration of high volume fraction CNTs into structure. Besides, CNTs morphology and orientation could be precisely controlled. Interfacial interaction between polymer and reinforcing element promoted the effective load transfer mechanisms benefiting either micromechanical interlocking, chemical bonding or Van der Waals bonding. The interaction between CNTs and polymer provided an increase in interfacial shear strength and contributed to the overall structure' performance under different loadings. In this thesis, a novel method to grow CNTs on polymeric nanofibrous substrates and to fabricate their thermoplastic nanoprepregs interleaved by these hierarchical nanocarpets was proposed. The growth of CNTs on polybenzimidazole (PBI) nanofibers were exploited to create conductive, strong and light weight interleaves. Nanofibers produced by electrospinning were optimized and catalysed with iron nitrate solutions containing transition metals providing carbon diffusion and solubility. As coating method to dope catalyst, immersion and dip-coating techniques were preferred. These different coating methods were assessed based on their ability to distribute transition metals onto nanofiber. The chemical vapour deposition (CVD) for the growth of CNTs was preferred due to its advantages such as; CNTs orientation control and high quality of CNTs. With the use of ethylene, helium and hydrogen gases, CNTs growth protocol was optimized. The orientation control of CNTs could be enhanced by aligned nanofibers as substrates. PBI/CNTs nanocarpets were then used as interleaves for the production of thermoplastic nanoprepregs. Thermoplastic nanoprepregs were prepared and characterized as potential interlayer element in laminated composites. The morphology, thermal stability and overall quality of CNTs were determined by SEM, TGA and Raman spectroscopy respectively. From morphological analysis, revealed that randomly oriented PBI nanofibers could not enable vertically aligned CNTs growth due to homogenously accumulated Fe+3 ions over nanofiber surface. Ig/Id ratio interpreted from Raman analysis was determined as 1 which referred as successful production of high quality CNTs grown onto nanofiber. The electrical conductivity of PBI/CNTs nanocarpets was calculated by 4 point probe conductivity instrument. Conductivity values of randomly oriented and aligned PBI/CNTs nanocarpets were 1.56±0.6 S/cm and 1.2±0.5 S/cm, respectively. The difference in the conductivity could be attributed to the reduced contact resistance between carbon nanotubes and well intersected CNTs network. The tensile performance of PBI/CNTs/PES nanoprepregs showed that tensile strength of PBI/CNTs/PES nanoprepregs was 412±13 MPa, where PBI/PES nanoprepregs had a tensile strength of 348±5 MPa. With the addition of CNTs onto nanofiber, tensile strength of nanoprepregs was enhanced by 18%. The reason behind this increase was mechanical interlocking and good load transfer between CNTs and PES resin.