Understanding the Role of Oxidative Debris on the Structure of Graphene Oxide Films at the Air-Water Interface: A Neutron Reflectivity Study

We address here the role of oxidation impurities on air the structure of graphene oxide films at the air-water interface by water specular neutron reflectivity (SNR). We study films of purified graphene oxide (PGO) and nonpurified graphene oxide in the two layers close-packed state. Nonpurified graphene oxide is constituted by graphene oxide (GO) layers with oxidation impurities adsorbed on the basal plan; while in PGO sheets, impurities are eliminated. SNR measurements show that GO films are formed by well-defined bilayers constituted by 2-3 layers of GO stacked in contact with air and a second layer of impurities submerged in the aqueous subphase. In contrast, PGO films are formed by a single layer in contact with air. We show for the first time that impurities constitute a layer submerged in the aqueous subphase, decrease the elasticity, and favor the collapse of graphene oxide films. Our results allow designing the surface properties of GO trapped at fluid interfaces.