The susceptibility to delamination is one of the main concerns in fiber reinforced polymer composites (FRPs). This work demonstrates improvements of 60% in Mode-I fracture toughness after integration of thin (~30 micron), continuous veils of carbon nanotubes (CNTs) directly deposited onto carbon fiber fabric as the CNT are drawn from the gas-phase using a semi-industrial process. A combination of optical imaging, scanning electron microscopy and a Raman spectroscopy provide a new rapid tool to unambiguously determine the crack propagation path by simple visual inspection of fracture surface. The results show that interlaminar crossing between CNT veil/CF interfaces is of paramount importance. The crack front alternatingly propagates above and below the CNT-toughened interlayer, significantly improving the fracture toughness of resultant laminates. This mechanism is strongly influenced by the method used to integrate the veils onto the CF. CNT veils directly deposited onto the fabrics as a low-density layer lead to large improvements in interlaminar properties, whereas compact CNT veils densified by solvent exposure prior to their integration in the lay-up act as defects.

This work presents a method to produce structural composites capable of energy storage. They are produced by integrating thin sandwich structures of CNT fiber veils and an ionic liquid-based polymer electrolyte between carbon fiber plies, followed by infusion and curing of an epoxy resin. The resulting structure behaves simultaneously as an electric double-layer capacitor and a structural composite, with flexural modulus of 60 GPa and flexural strength of 153 MPa, combined with 88 mF/g of specific capacitance and the highest power (30 W/kg) and energy (37.5 mWh/kg) densities reported so far for structural supercapacitors. In-situ electrochemical measurements during 4-point bending show that electrochemical performance is retained up to fracture, with minor changes in equivalent series resistance for interleaves under compressive stress. En route to improving interlaminar properties we produce grid-shaped interleaves that enable mechanical interconnection of plies by the stiff epoxy. Synchrotron 3D X-ray tomography analysis of the resulting hierarchical structure confirms the formation of interlaminar epoxy joints. The manuscript discusses encapsulation role of epoxy, demonstrated by charge-discharge measurements of composites immersed in water, a deleterious agent for ionic liquids. Finally, we show different architectures free of current collector and electrical insulators, in which both CNT fiber and CF act as active electrodes.

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