Heterogenity of graphite oxide particles obtained with wet oxidative exfoliation

Wet oxidative exfoliation of graphite is one of the most frequently applied techniques to obtain aqueous dispersions of hydrophilic graphene derivatives as required, e.g., in 3D printing, wet spinning or film casting. Due to the harsh conditions of the process, the resulting suspension is a mixture of particles with a wide distribution range both of physical dimensions and chemical properties. An aqueous graphite oxide suspension was obtained by an improved Hummers method and separated into five fractions by controlled centrifugation. The fractions were characterized and compared by various methods, revealing their diversity in size, chemical properties and application-related viscosity. The characterization methods (powder XRD, Raman spectroscopy, ATR-FTIR spectroscopy, XPS, potentiometric titration, rheology) exhibited subtle but measurable differences that exceeded the standard deviation of the techniques employed, but no systematic trend was found across the fractions in any of the properties investigated. The conditions of our centrifugal separation hardly meet the constrains of the ideal of Stokes's law, the polydispersity of the high aspect ratio particles as well as their concentration close to the percolation limit challenge the independent sedimentation of the platelets.