• DOI:10.1039/c6sm00621c
• Corpus ID: 25513764

Mesoscopic simulations of hydrophilic cross-linked polycarbonate polyurethane networks: structure and morphology.

@article{Iype2016MesoscopicSO,
  title={Mesoscopic simulations of hydrophilic cross-linked polycarbonate polyurethane networks: structure and morphology.},
  author={Eldhose Iype and A C C Esteves and Gijsbertus de With},
  journal={Soft matter},
  year={2016},
  volume={12 22},
  pages={
          5029-40
        }
}

• E. Iype, A. Esteves, G. de With
• Published 1 June 2016
• Materials Science
• Soft matter

Polyurethane (PU) cross-linked networks are frequently used in biomedical and marine applications, e.g., as hydrophilic polymer coatings with antifouling or low-friction properties and have been reported to exhibit characteristic phase separation between soft and hard segments. Understanding this phase-separation behavior is critical to design novel hydrophilic polymer coatings. However, most of the studies on the structure and morphology of cross-linked coatings are experimental, which only assess the phase separation via indirect methods. Herein we present a mesoscopic simulation study of the network characteristics of model hydrophilic polymer networks, consisting of PU with and without methyl-polyethylene glycol (mPEG) dangling chains. The systems are analyzed using a number of tools, such as the radial distribution function, the cross-link point density distribution and the Voronoi volume distribution (of the cross-linking points). The combined results show that the cross-linked networks without dangling chains are rather homogeneous but contain a small amount of clustering of cross-linker molecules. A clear phase separation is observed when introducing the dangling chains. In spite of that, the amount of cross-linker molecules connected to dangling chains only, i.e., not connected to the main network, is relatively small, leading to about 3 wt% extractables. Thus, these cross-linked polymers consist of a phase-separated, yet highly connected network. This study provides valuable guidelines towards new self-healing hydrophilic coatings based on the molecular design of cross-linked networks in direct contact with water or aqueous fluids, e.g., as anti-fouling self-repairing coatings for marine applications.