Chemical Oxidation of Graphite: Evolution of the Structure and Properties

Graphene oxide is a complex material whose synthesis is still incompletely understood. To study the time evolution of structural and chemical properties of oxidized graphite, samples at different temporal stages of oxidation were selected and characterized through a number of techniques: X-ray photoelectron spectroscopy for the content and bonding of oxygen, X-ray diffraction for the level of intercalation, Raman spectroscopy for the detection of structural changes, electrical resistivity measurements for probing charge localization on the macroscopic scale, and scanning transmission electron microscopy for the atomic structure of the graphene oxide flakes. We found a nonlinear behavior of oxygen uptake with time where two concentration plateaus were identified: Uptake reached 20 at % in the first 15 min, and after 1 h a second uptake started, reaching a highest oxygen concentration of >30 at % after 2 h of oxidation. At the same time, the interlayer distance expanded to more than twice the value of graph...