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 the structure of graphene oxide films at the air-water interface by specular neutron reflectivity (SNR). We study films of purified graphene oxide (PGO) and nonpurified graphene oxide in the close-packed state. Nonpurified graphene oxide is constituted by graphene oxide (GO) layers with oxidation impurities adsorbed on the basal plane, 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.