A conductive polymer film containing pristine graphene was prepared by designing a polysiloxane-based stabilizer for graphene. The stabilizer was prepared by grafting 1-ethynylpyrene to the backbone of a poly(dimethylsiloxane)-co-(methylhydrosiloxane) (PDMS-PHMS) random copolymer by Pt-catalyzed hydrosilylation with a SiH-ethynyl ratio of 1.0 : 1.3. The resulting copolymer was able to stabilize pristine graphene in chloroform solution viaπ-π interactions between the pyrene groups and graphene sheets. TEM and SEM images show a homogeneous distribution of the graphene in cast films deposited from chloroform. The conductivity of a graphene/PDMS film prepared from copolymer with a 1.7 vol.% graphene loading was measured as 220 S m(-1) after the removal of unbound polymer by a simple separation technique. With a SiH-ethynyl ratio of 1.7 : 1.0, the copolymer self-crosslinked at 110 °C in the presence of adventitious moisture, providing a straightforward route to incorporate graphene into silicone elastomers. The crosslinking process (with and without added graphene) was characterized by FT-IR spectroscopy and by swelling and extraction of the obtained networks. Again, unbound polymer removal increases the conductivity of the composite.
We describe the first preparation of polymer-supported pristine graphene thin films with dramatically different electrical conductivities on the top and bottom surfaces. Pyrene-functional stabilizers based on polystyrene or poly(methyl methacrylate) were first synthesized by copolymerization of their monomers with 1-pyrenemethyl methacrylate. Stable dispersions of pristine graphene nanosheets were prepared by sonication of graphite in chloroform solutions of the pyrene-functional copolymers. Vacuum filtration of the polymer-stabilized graphene dispersions through a porous PTFE filter produces films with an internal gradient in nanosheet concentration. This gradient graphene concentration results in an electrically conductive, graphene-rich surface on one side of the composite film and a nonconductive, polymer-rich surface on its other side. Electrical conductivities ranging from 60 to 194 S/m are measured on the graphene-rich surface, which are among the highest conductivities reported for pristine graphene/polymer composites. Through scanning electron microscopy and secondary ion mass spectrometry characterization, these films were found to contain three distinct layers: a polymer-rich top surface, a transition layer with a gradient in nanosheet concentration, and a buckypaper-like bottom layer consisting of densely packed, highly oriented graphene nanosheets. The gradient structure of these films and their Janus-like electrical conductivity has potential applications in graded coatings for radiofrequency and optical devices.
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