Double Percolation of Poly(lactic acid)/Low-Density Polyethylene/Carbon Nanotube (PLA/LDPE/CNT) Composites for Force-Sensor Application: Impact of Preferential Localization and Mixing Sequence

This study explores the enhancement of electrical conductivity in polymer composites by incorporating carbon nanotubes (CNTs) into a co-continuous poly(lactic acid)/low-density polyethylene (PLA/LDPE) blend, creating a double percolation structure. Theoretical thermodynamic predictions indicate that CNTs preferentially localize in the LDPE phase. The percolation threshold of CNTs in the PLA/LDPE/CNT composites was 0.208 vol% (5.56 wt%), an 80% reduction compared to the LDPE/CNT composite, due to the double percolation structure. This thermodynamic migration of CNTs from PLA to LDPE significantly enhanced conductivity, achieving a 13.8-fold increase at a 7.5 wt% CNT loading compared to the LDPE/CNT composite. The localization of CNTs was driven by thermodynamic, kinetic, and rheological factors, with viscosity differences between PLA and LDPE causing dense CNT aggregation in LDPE. Initial contact of CNTs with PLA reduced aggregation, allowing PLA to infiltrate CNT aggregates during melt-mixing, which influenced the final morphology and electrical conductivity. These findings provide new insights into the fabrication of conductive polymer composites for force sensor applications.