The Micro-Capacitance Enhancement of Polyionic Liquids Grafted Onto Carbon Nanotubes on the Piezoelectric Properties of Poly(Vinylidene Fluoride) Films and Their Sensor Applications

The increased micro-capacitance of a poly (vinylidene fluoride) (PVDF) matrix can effectively improve the piezoelectric properties of the composite material. This work used chemically modified carbon nanotubes (CNTs) as the main reinforcement material. Atom transfer radical polymerization (ATRP) was used to graft polyionic liquids (PILs) with different hydrophilic anions to the CNTs' surfaces. Solution casting and compressive melt molding were used to prepare the PVDF-composite piezoelectric films. Micro-capacitance formed by the PIL grafted CNTs dispersed well in the PVDF matrix, and their effects on the crystalline form and piezoelectric properties were studied. The hydrophobic hexafluorophosphate anion (-PF6-) can significantly improve the CNTs dispersion and enhance the micro-capacitance formation in the PVDF matrix. During solution crystallization, the synergistic effect of CNTs and PIL on the PVDF and the solvent effect made the content of beta phase of PVDF/CNTs@PIL-PF6 film reach 80.2%, resulting in a high dielectric constant of 188 and a piezoelectric coefficient of 36. In the process of melt crystallization, due to shear stretching and extrusion, the CNTs@PIL-PF6 had an obvious nucleation effect on the polar crystalline phase of PVDF, with a beta phase content up to 99.3%, leading to the higher dielectric constant of 530 and the piezoelectric coefficient of 31. The current discovery provides a development direction for smart piezoelectric polymer matrix composites, which have great potential in preparing piezoelectric energy storage materials.