Piezoelectric performance of lead-free PDMS/CNT/BaTiO₃ piezocomposites with imperfect interphases and CNT agglomerations

Three-dimensional (3D) printable lead-free piezocomposites offer scalable and environmentally friendly solutions in many engineering applications. Typically, the composite system consists of polymeric matrices reinforced with active polycrystalline particles, and possibly nanoadditives. The presence of interfacial inclusion/matrix damage could not only compromise the structural integrity of the component but also significantly alter its ability to act as functional smart materials. In addition, both the agglomeration of the nanoadditives, such as carbon nanotubes (CNTs), and the degree of polarization could also affect the electromechanical behavior of the composite. In this paper, we develop a computational micromechanical model for the study of the influence of three types of internal defects on the piezoelectric performance of such composites. We investigate the influence of (a) the texture of the active phase, which is linked to the degree of polarization; (b) the effect of agglomerations of the CNTs; and (c) the presence of damage in the inclusion/matrix interphase region. Performance is assessed through the macroscopic response in various figures of merit. This work provides numerical evidence that the effective piezoelectric constants related to normal strain modes are strongly affected by the presence of damage in the interphase. Instead, the piezoelectric constant related to the shear strain remains unchanged by interfacial damage. Near the percolation threshold of the CNTs, piezocomposites exhibit a notable improvement in the piezoelectric response compared to the composite without nanomodification, as noted in previous works. Interestingly, this trend also applies in the presence of interfacial damage, and it is described in this work. The piezoelectric performance also depends on the texture of the active particles. We find, under some simplifications, the optimal orientation for the crystallites, and we find how the texture changes the performance in the presence of damage. Regarding energy harvesting applications, optimal energy conversion efficiency has been observed for polycrystalline inclusions that resembles a highly oriented single crystal and CNT volume fraction of 60 % of percolation threshold. This is a quite surprising result since the optimal is usually expected for volume fractions very close to percolation and active inclusions with some orientational dispersion. The optimal CNT volume fraction depends on the presence of interfacial damage. Under perfect interface conditions, the energy conversion efficiency is improved with the presence of CNT agglomerations. Under imperfect interface conditions, there is no enhancement due to the addition of CNT.