Abstract
Polymer dielectrics offer key advantages over their ceramic counterparts such as flexibility, scalability, low cost, and high breakdown voltages. However, a major drawback that limits more widespread application of polymer dielectrics is their temperature-dependent dielectric properties. Achieving dielectric constants with low/zero-temperature coefficient (L/0TC) over a broad temperature range is essential for applications in diverse technologies. Here, we report a hybrid filler strategy to produce polymer composites with an ultrawide L/0TC window of dielectric constant, as well as a significantly enhanced dielectric value, maximum energy storage density, thermal conductivity, and stability. By creating a series of percolative polymer composites, we demonstrated hybrid carbon filler based composites can exhibit a zero-temperature coefficient window of 200 °C (from -50 to 150 °C), the widest 0TC window for all polymer composite dielectrics reported to date. We further show the electric and dielectric temperature coefficient of the composites is highly stable against stretching and bending, even under AC electric field with frequency up to 1 MHz. We envision that our method will push the functional limits of polymer dielectrics for flexible electronics in extreme conditions such as in hybrid vehicles, aerospace, power electronics, and oil/gas exploration.