In this work, the arising of stick-slip dissipation as well as the global mechanical response of carbon nanotube (CNT) nanocomposite films are tailored by exploiting a three-phase nanocomposite. The three phases are represented by the CNTs, a polymer coating localized on the CNTs surface and a hosting matrix. In particular, a polystyrene (PS) layer coats multi-walled carbon nanotubes (MWNTs) that are randomly dispersed in a polyimide (PI) matrix. The coating phase is strongly bonded to the CNTs outer sidewalls ensuring the effectiveness of the load transfer mechanism and reducing the material damping capacity. The coating phase can be thermally-activated to modify, and in particular, decrease the CNT-matrix interfacial shear strength (ISS) thus facilitating the stick-slip onset in the nanocomposite. The ISS decrease finds its roots in a partial degradation of the coating phase and, in particular, in the formation of voids. By weakening the CNT/polymer interfacial region, a significant enhancement in the material damping capacity is observed. An extensive experimental campaign consisting of monotonic and cyclic tensile tests proved the effectiveness of this novel multi-phase material design.

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