Universal Control on Pyroresistive Behavior of Flexible Self‐Regulating Heating Devices

Abstract Smart heating devices with reliable self‐regulating performances and high efficiency, combined with additional properties like mechanical flexibility, are of particular interest in healthcare, soft robotics, and smart buildings. Unfortunately, the development of smart heaters necessitates managing normally conflicting requirements such as good self‐regulating capabilities and efficient Joule heating performances. Here, a simple and universal materials design strategy based on a series connection of different conductive polymer composites (CPC) is shown to provide unique control over the pyroresistive properties. Hooke's and Kirchhoff's laws of electrical circuits can simply predict the overall pyroresistive behavior of devices connected in series and/or parallel configurations, hence providing design guidelines. An efficient and mechanically flexible Joule heating device is hence designed and created. The heater is characterized by a zero temperature coefficient of resistance below the self‐regulating temperature, immediately followed by a large and sharp positive temperature coefficient (PTC) behavior with a PTC intensity of around 10⁶. Flexibility and toughness is provided by the selected elastomeric thermoplastic polyurethane (TPU) matrix as well as the device design. The universality of the approach is demonstrated by using different polymer matrices and conductive fillers for which repeatable results are consistently obtained.