Article abstract


Nature Materials 5, 229 - 233 (2006)
doi:10.1038/nmat1582

Subject Categories: Composites | Polymers | Nanoscale materials

Entropy-driven segregation of nanoparticles to cracks in multilayered composite polymer structures

Suresh Gupta1,3, Qingling Zhang1,3, Todd Emrick1, Anna C. Balazs2 and Thomas P. Russell1


Multilayer composites, which combine ductile polymers with brittle films, constitute vital components for optical communications, microelectronics and bio-engineering applications. However, crack formation is a critical problem in these materials; thus, designing layered systems that can respond to environmental changes and undergo self-healing is particularly important for a range of technologies. Here, nanoparticles dispersed in a polymer matrix were found to migrate to a crack generated at the interface between the polymer and a glassy layer. Segregation of the nanoparticles to the crack depended on both the enthalpic and entropic interactions between the polymer and nanoparticles. In particular, poly(ethylene oxide)-covered 5.2-nm spherical nanoparticles in a poly(methyl methacrylate) matrix diffused to cracks in the adjoining silicon oxide layer, whereas tri-n-octylphosphine oxide-covered nanoparticles did not. These results point to a simple means of fabricating systems that can self-heal, improving the durability of multilayered systems, or form the basis for auto-responsive materials.

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  1. Polymer Science and Engineering Department, University of Massachusetts, Amherst, Massachusetts 01003, USA
  2. Department of Chemical and Petroleum Engineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, USA
  3. These authors contributed equally to this work

Correspondence to: Todd Emrick1 e-mail: tsemrick@mail.pse.umass.edu

Correspondence to: Thomas P. Russell1 e-mail: russell@mail.pse.umass.edu

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