Large-Area Chemically Modified Graphene Films: Electrophoretic Deposition and Characterization by Soft X-ray Absorption Spectroscopy

A facile, rapid. and scalable electrophoretic deposition approach is developed for the fabrication of large-area chemically derived graphene films on conductive substrates based on the electrophoretic deposition of graphene oxide and reduced graphene oxide components. Two distinctive approaches for fabricating conformal graphene films are developed. In the first approach, graphene oxide sheets are electrophoretically deposited from an aqueous solution after the oxidation of graphite to graphite oxide and the subsequent exfoliation of graphite oxide to graphene oxide. Next, the graphene oxide films are reduced via dip-coating in an aqueous Solution of hydrazine. In the second approach, graphene oxide is reduced to graphene nanosheets in a strongly alkaline Solution and the reduced graphene sheets are directly electrophoretically deposited onto conductive substrates. The film thickness can be modified by the deposition time and the obtained films span several square millimeters in area. Near-edge X-ray absorption fine structure (NEXAFS) spectroscopy is used to Study the Surface chemistry. electronic band structure. and degree of alignment of the electrophoretically deposited films. Polarized NEXAFS measurements verify the presence of epoxide surface functionalities on the graphene basal planes and indicate significant recovery of extended pi-bonded networks upon defunctionalization by hydrazine treatment. These measurements further indicate significantly improved alignment of the graphene sheet components of the films parallel to the substrate surface when defunctionalization is performed prior to electrophoretic deposition.