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In this paper, we propose a facile approach to the management of graphene oxide (GO) chemistry via its synthesis using KMnO 4 /K 2 Cr 2 O 7  oxidizing agents at different ratios. Using Fourier Transformed Infrared Spectroscopy, X-ray Photoelectron Spectroscopy, and X-ray Absorption Spectroscopy, we show that the number of basal-plane and edge-located oxygenic groups can be controllably tuned by altering the KMnO 4 /K 2 Cr 2 O 7  ratio. The linear two-fold reduction in the number of the hydroxyls and epoxides with the simultaneous three-fold rise in the content of carbonyls and carboxyls is indicated upon the transition from KMnO 4  to K 2 Cr 2 O 7  as a predominant oxidizing agent. The effect of the oxidation mixture’s composition on the structure of the synthesized GOs is also comprehensively studied by means of X-ray diffraction, Raman spectroscopy, transmission electron microscopy, atomic-force microscopy, optical microscopy, and the laser diffraction method. The nanoscale corrugation of the GO platelets with the increase of the K 2 Cr 2 O 7  content is signified, whereas the 10–100 μm lateral size, lamellar, and defect-free structure is demonstrated for all of the synthesized GOs regardless of the KMnO 4 /K 2 Cr 2 O 7  ratio. The proposed method for the synthesis of GO with the desired chemistry opens up new horizons for the development of graphene-based materials with tunable functional properties.

Graphene Oxide Chemistry Management via the Use of KMnO4/K2Cr2O7 Oxidizing Agents