High-Temperature Response Polylactic Acid Composites by Tuning Double-Percolated Structures

Due to the properties of a positive temperature coefficient (PTC) effect and a negative temperature coefficient (NTC) effect, electrically conductive polymer composites (CPCs) have been widely used in polymer thermistors. A dual percolated conductive microstructure was prepared by introducing the polybutylene adipate terephthalate phase (PBAT) into graphene nanoplatelets (GNPs)-filled polylactic acid (PLA) composites, intending to develop a favorable and stable PTC material. To achieve this strategy, GNPs were selectively distributed in the PBAT phase by injection molding. In this study, we investigated the crystallization behavior, electrical conductivity, and temperature response of GNP-filled PLA/PBAT composites. The introduction of GNPs into PLA significantly increased PLA crystallization capacity, where the crystallization onset temperature (To) is raised from 116.7 °C to 134.7 °C, and the crystallization half-time (t1/2) decreases from 35.8 min to 27.3 min. The addition of 5 wt% PBAT increases the electrical conductivity of PLA/PBAT/GNPs composites by almost two orders of magnitude when compared to PLA/GNPs counterparts. The temperature of the heat treatment is also found to play a role in affecting the electrical conductivity of PLA-based composites. Increasing crystallinity is favorable for increasing electrical conductivity. PLA/PBAT/GNPs composites also show a significant positive temperature coefficient, which is reflected in the temperature–electrical resistance cycling tests.