No abstract

Self-assembled alkane layers are introduced between graphene layers to physically block nanometer size defects in graphene and lateral gas pathways between graphene layers. A welldefined hexatriacontane (HTC) monolayer on graphene could cover nanometer-size defects because of the flexible nature and strong intermolecular van der Waals interactions of alkane, despite the roughness of graphene. In addition, HTC multilayers between graphene layers greatly improve their adhesion. This indicates that HTC multilayers between graphene layers can effectively block the lateral pathway between graphene layers by filling open space with close-packed self-assembled alkanes. By these mechanisms, alternately stacked composites of graphene and self-assembled alkane layers greatly increase the gas-barrier property to a water vapor transmission rate (WVTR) as low as 1.2 × 10 −3 g/(m 2 day), whereas stacked graphene layers generally show a WVTR < 0.5 g/ (m 2 day). Furthermore, the self-assembled alkane layers have superior crystallinity and wide bandgap, so they have little effect on the transmittance.

Defects on graphene over a micrometer in size were selectively blocked using polyvinyl alcohol through the formation of hydrogen bonding with defects. Because this hydrophilic PVA does not prefer to be located on the hydrophobic graphene surface, PVA selectively filled hydrophilic defects on graphene after the process of deposition through the solution. The mechanism of the selective deposition via hydrophilic–hydrophilic interactions was also supported by scanning tunneling microscopy and atomic force microscopy analysis of selective deposition of hydrophobic alkanes on hydrophobic graphene surface and observation of PVA initial growth at defect edges.