Surface Roughness Enhances Self-Nucleation of High-Density Polyethylene Droplets Dispersed within Immiscible Blends

Macromolecules. 2022 Feb 22;55(4):1412-1423. doi: 10.1021/acs.macromol.1c02487. Epub 2022 Feb 11.

Abstract

Highly linear or high-density polyethylenes (HDPEs) have an intrinsically high nucleation density compared to other polyolefins. Enhancing their nucleation density by self-nucleation is therefore difficult, leading to a narrow self-nucleation Domain (i.e., the so-called Domain II or the temperature Domain where self-nuclei can be injected into the material without the occurrence of annealing). In this work, we report that when HDPE is blended (up to 50%) with immiscible matrices, such as atactic polystyrene (PS) or Nylon 6, its self-nucleation capacity can be greatly increased. In addition, temperatures higher than the equilibrium melting temperature of the HDPE phase are needed to erase the significantly enhanced crystalline memory in the blends. Morphological evidence gathered by Scanning and Transmission Electron Microscopies (SEM and TEM) indicates that these unexpected results can be explained by the modification of the interface between blend components. The filling of the solid HDPE surface asperities by the low viscosity polystyrene during heating to the self-nucleation temperature, or the crystallization of the matrix in the case of Nylon 6, enhances the interface roughness between the two polymers in the blends. Such rougher interfaces can remarkably increase the self-nucleation capacity of the HDPE phase via surface nucleation.