Polymer-based materials with positive temperature coefficients (PTC) are regarded as potential candidates for electrical heating elements in a wide range of applications, such as wearable electronics, soft robots, and smart skin. They offer many advantages over ceramic or metal oxide-based composites, including low resistance at room temperature, excellent flexibility and processability, and low cost. However, the electrical resistance instability and poor reproducibility have limited their use in practical applications. In this work, we prepared carbon blacks-reinforced high-density polyethylene nanocomposites (CBs-HDPE) loaded with polar additives (polyols or ionomers), which were subsequently subjected to electron beam (EB) irradiation to explore their PTC behaviors. We found that the EB-treated nanocomposites exhibited PTC behaviors, while the untreated samples showed negative temperature coefficients. Further, EB-ionomer-CBs-HDPE showed the highest PTC intensity of 3.01 Ω·cm, which was ∼35% higher than that of EB-CBs-HDPE. These results suggested that the EB irradiation enabled a specific volume expansion behavior via enhanced crosslinking among CBs, polar additives, and HDPE, inhibiting the formation of conductive networks in the nanocomposites. Thus, it can be concluded that polar additives and further EB irradiation played an important role in enhancing the PTC performances. We believe the findings provide crucial insight for designing carbon-polymer nanocomposites with PTC behaviors in various self-regulating heating devices.
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