Electroanalytical Sensing Properties of Pristine and Functionalized Multilayer Graphene

Abstract

This paper describes the heterogeneous electron transfer (ET) properties of high-quality multilayer graphene (MLG) films grown using chemical vapor deposition (CVD) on nickel and transferred to insulating poly(ethylene terephthalate) (PET) sheets. An oxygen plasma treatment is used to enhance the ET properties of the films by generating oxygenated functionalities and edge-plane sites and defects. Scanning electron microscopy (SEM), Raman, and X-ray photoelectron spectroscopy (XPS) along with voltammetry of the standard redox probes [Ru(NH3)6]3+/2+, [Fe(CN)6]3–/4–, and Fe3+/2+ are used to demonstrate this effect. The biologically relevant molecules dopamine, NADH, ascorbic acid, and uric acid are employed to show the improved sensing characteristics of the treated films. Control experiments involving commercially available edge-plane and basal-plane pyrolytic graphite (EPPG and BPPG) electrodes help to explain the different responses observed for each probe, and it is shown that, in certain cases, treated MLG provides a viable alternative to EPPG, hitherto considered to be the “best-case scenario” in carbon electrochemistry. This is the first comprehensive study of the electroanalytical properties of pristine and functionalized CVD-grown MLG, and it will serve as an important benchmark in the clarification of ET behavior at graphene surfaces, with a view to the development of novel electrochemical sensors.