Tuning the mechanical properties of graphene oxide paper and its associated polymer nanocomposites by controlling cooperative intersheet hydrogen bonding

Owen C. Compton, Steven W. Cranford, Karl W. Putz, Zhi An, L. Catherine Brinson*, Markus J. Buehler, Sonbinh T. Nguyen

*Corresponding author for this work

Research output: Contribution to journalArticle

307 Scopus citations

Abstract

The mechanical properties of pristine graphene oxide paper and paper-like films of polyvinyl alcohol (PVA)-graphene oxide nanocomposite are investigated in a joint experimental-theoretical and computational study. In combination, these studies reveal a delicate relationship between the stiffness of these papers and the water content in their lamellar structures. ReaxFF-based molecular dynamics (MD) simulations elucidate the role of water molecules in modifying the mechanical properties of both pristine and nanocomposite graphene oxide papers, as bridge-forming water molecules between adjacent layers in the paper structure enhance stress transfer by means of a cooperative hydrogen-bonding network. For graphene oxide paper at an optimal concentration of ∼5 wt % water, the degree of cooperative hydrogen bonding within the network comprising adjacent nanosheets and water molecules was found to optimally enhance the modulus of the paper without saturating the gallery space. Introducing PVA chains into the gallery space further enhances the cooperativity of this hydrogen-bonding network, in a manner similar to that found in natural biomaterials, resulting in increased stiffness of the composite. No optimal water concentration could be found for the PVA-graphene oxide nanocomposite papers, as dehydration of these structures continually enhances stiffness until a final water content of ∼7 wt % (additional water cannot be removed from the system even after 12 h of annealing).

Original languageEnglish (US)
Pages (from-to)2008-2019
Number of pages12
JournalACS nano
Volume6
Issue number3
DOIs
StatePublished - Mar 27 2012

Keywords

  • graphene oxide
  • graphene oxide paper
  • mechanical properties
  • molecular dynamics simulations
  • polymer nanocomposite

ASJC Scopus subject areas

  • Engineering(all)
  • Materials Science(all)
  • Physics and Astronomy(all)

Fingerprint Dive into the research topics of 'Tuning the mechanical properties of graphene oxide paper and its associated polymer nanocomposites by controlling cooperative intersheet hydrogen bonding'. Together they form a unique fingerprint.

  • Cite this