Synthesis and Applications of Large Area Graphene-Based Electrode Systems.

摘要

Graphene is a single sheet of carbon atoms with outstanding electrical and physical properties and being exploited for applications in electronics, sensors, fuel cells, photovoltaics and energy storage. However, practical designs of graphene-based electrode systems and related experimental implementations are required to realize their widespread applications in nano- to bioelectronics. In this dissertation, different graphene-based electrode systems having metallic and semiconducting properties are synthesized optimizing process conditions. Also realized is the potential of the fabricated electrode systems by applying them in practical applications such as sensor devices and fuel cells.;The zero bandgap of semimetal graphene still limits its application as an effective field-effect transistor device or a chemiresistor sensor operating at room temperature. It has been shown theoretically and experimentally that graphene nanoribbons (GNRs) or nanomeshes (GNMs) can attain a bandgap that is large enough for a transistor device, and hence would show high sensitivity to various gaseous species or biomolecules. Large-area mono- and bilayer graphene films are synthesized by a simple chemical vapor deposition (CVD) technique depending on the carbon precursors such as methane, acetylene and ethanol, and the results are compared using optical microscopy (OM), Raman spectroscopy, high-resolution transmission electron microscopy (HRTEM) and x-ray photoelectron spectroscopy (XPS). A simple reactive ion etching (RIE) combined with well-established nanosphere lithography is performed on the synthesized CVD-grown monolayer graphene platform to fabricate large area GNMs with specific dimension and periodicity. The fabricated GNMs chemiresistor sensor devices show excellent sensitivity towards NO2 and NH 3, significantly higher than their film counterparts. The GNM sensor devices exhibit sensitivities of about 4.32%/ppm (parts-per-million) in NO 2 and 0.71%/ppm in NH3 with estimated limit of detections of 15 ppb (parts-per billion) and 160 ppb, significantly lower than Occupational Safety and Health Administration (OSHA) permissible exposure limits of 5 ppm (NO2) and 50 ppm (NH3), respectively. The demonstrated studies on the sensing properties of graphene nanomesh would essentially lead further improvement of it's sensitivity and selectivity as a potential sensor material.;Furthermore, a three-dimensional (3D) carbon electrode in the form of vertically aligned carbon nanotubes (CNTs) on a graphene floor is applied as a supporting electrode for platinum (Pt) nanoflowers electrocatalysts in methanol oxidation as well as in nonenzymatic sensing of blood glucose. Experimental results demonstrate an enhanced efficiency of the 3D graphene-carbon nanotubes hybrid film, as catalyst support, for methanol oxidation with regard to electroactive surface area, forward anodic peak current density, onset oxidation potential, diffusion efficiency and the ratio of forward to backward anodic peak current density (If/Ib). Also, the developed nonenzymatic 3D carbon hybrid sensor responded linearly to the physiological glucose concentration ranging from 1 to 7 mM (R2 = 0.978) with a sensitivity of 11.06 muA mM-1cm-2.