The design and fabrication of highly piezoelectric polymeric composites and their use in responsive devices

In this work, novel approaches to the design of highly piezoelectric and flexible polymer composites were explored. Diverging from past work focused on the addition of piezoelectric particles into polymer matrices, this research explores the ability to increase the piezoelectric performance of a host polymer through the incorporation of charge via polarizable, organic particles. The ability to insert charge into polymers, known as electrets, is well documented but widely considered impractical because of the low lifetime and temperature resistance of the inserted charge. Through the addition of particles that are polarizable, charge can be inserted into a system in a stable manner that results in highly charged materials with long lifetimes. Here, carbon structures, such as Buckminsterfullerenes (C60) and single-walled nanotubes (SWNTs), were composited into poly(vinylidene difluoride) at very low loading levels (0.05-0.25 wt%), resulting in the ability to insert stable charge into the system. We show that these highly charged systems can result in a doubling of the piezoelectric response of the host polymer when optimized. The low amount of nanoparticle filler required to improve these materials allows for the advantageous properties of the polymer matrix such as flexibility and compliance to be preserved, enabling highly piezoelectric and flexible system.;This dissertation outlines research efforts towards the design and fabrication of 1) polymer composites with high piezoelectric response, 2) piezoelectric composites with increased operating temperatures, 3) motion control devices that incorporate piezoelectric materials and shape memory polymers, and 4) artificial muscles with piezoelectric polymers. The piezoelectric polymer composites developed in this work have potential to be utilized as highly efficient, flexible energy harvesters that can be used to capture ambient energy from environmental vibrations and motion from the human body. As actuators, these materials may find use as rapid-response muscle replacements in legs, arms, fingers, or toes. As sensors, such devices may provide electrical impulses capable of sensing small vibrations due to structural damage or movements. There is a wide range of applications for flexible piezoelectric materials that will continue to expand as technologies in monitoring, energy harvesting, and motion control continue to develop.