Graphene-based Material Systems for Nanoelectronics and Energy Storage Devices
- Author(s): Guo, Shirui
- Advisor(s): Ozkan, Mihri
- Ozkan, Cengiz S
- et al.
Graphene is an allotrope of carbon in two-dimensional crystal form that has extraordinary electrical and optical properties. In this dissertation, we present the use of graphene in applications for chemical sensors, photovoltaics and supercapacitors.
Firstly, carrier transport properties of single layer graphene films grown via chemical vapor deposition technique are tuned with functionalized molecules, polymers and inorganic nanoparticles. For example, cylindrical microdomains of polystyrene-4-polyvinylpyridine (PS-P4VP) block-copolymers (BCP) on graphene film provide spatial doping effects due to two distinct functional groups. Further, preferred interactions between CFx or fluorine radicals and BCP micro domains on graphene introduce localized doping of graphene film leading to controlling of Dirac point shift. Interaction between graphene and inorganic nanoparticles is studied by using CdSe quantum dots as a model system. Femtosecond time-resolved spectroscopy allowes us to demonstrate for the first time fast interfacial charge transfer for such systems in the picosecond and in the hundreds of femtosecond time domains, which also demonstrates high potential for photoelectrochemical cell.
Secondly, graphene field effect transistors (GFET) as single strand DNA sensors are fabricated and detection limit as low as 3×10-9 M is demonstrated. Assembled BCP film on GFET sensor improved the sensor's stability and selectivity. The orientation and periodicity of the resulting cylindrical microdomains of BCP can facilitate the selective sensing property. With protective layer of BCP, sensor's stability under ambient atmosphere is improved up to 4 months.
Thirdly, two different types of carbon nanotubes (CNT)/graphene hybrids are synthesized and used in fabrication of supercapacitors. The first type hybrid is graphene and vertically aligned carbon nanotubes which is successfully grown via one step chemical vapor deposition method. Our custom seamless growth method for such hybrids provides an attractive pathway for the fabrication of novel 3-Dimensional hybrid nanostructures. The second type hybrid is graphene oxide (GO) and SWCNT composite ink (GO-SWCNT ink). SWCNTs are dispersed using a GO aqueous solution (2mg/ml) with sonication support to achieve a SWCNT concentration of 12mg/ml, the highest reported value so far without surfactant assistance. Paper based electrodes for supercapacitors are fabricated using GO-SWCNT composite ink via dip casting method. By employing different concentrations of SWCNT inside the ink, supercapacitors demonstrated different capacitance values. The highest value of specific capacitance reaches up to 295 F/g at a current density of 0.5A/g with a GO/SWCNT weight ratio of 1:5. The cycling stability for the GO-SWCNT paper electrode supercapacitors indicates capacitance retention of 85% over 60,000 cycles.
Finally, engineered interactions between nanomaterials, polymers, molecules and graphene/carbon nanotube can lead to the development of new types of devices for myriad applications.