A New Route to Tune the Electrical Properties of Graphene Oxide: A Simultaneous, One-Step N-Doping and Reduction as a Tool for Its Structural Transformation

Abstract

The presence of secondary electromagnetic waves (EMWs) results in EMW pollution and a large need for EMW-shielding materials. Therefore, new, lightweight, flexible, chemically resistant, and durable EMW shielding materials are demanded, while graphene and its derivatives meet the above-mentioned requirements. Among graphene derivatives, N-doped graphene exhibits promising electrical properties for shielding applications, although achieving sufficient N-incorporation in the graphene sheets remains a challenge. Herein, we produced graphene oxide using the modified Hummers' method (GO) and the electrochemical exfoliation of highly ordered pyrolytic graphite. These two GO samples were thermally treated at 500 °C and 800 °C under a pure NH3 gas for 1 h. UV-Vis, infrared, and Raman spectroscopies and X-ray diffraction, elemental, and thermogravimetric analyses were used to investigate the structural properties of modified GO. One of the highest levels of N-doping of GO was measured (11.25 ± 0.08 at%). The modification under a NH3 atmosphere leads to simultaneous N-doping and reduction of graphene, resulting in the formation of electrically conductive and EMW shielding materials. Density functional theory (DFT) revealed the effect of heteroatoms on the energy band gap of GO. The cluster corresponding to N-doped rGO had a reduced bandgap of 0.77 eV.