Jellyfish-like few-layer graphene nanoflakes: high paramagnetic response alongside increased interlayer interaction

Abstract

Abstract Jellyfish-like graphene nanoflakes (GNF), prepared by hydrocarbon pyrolysis, are studied with electron paramagnetic resonance (EPR) method. The results are supported by X-ray photoelectron spectroscopy (XPS) data. Oxidized (GNFox) and N-doped oxidized (N-GNFox) flakes exhibit an extremely high EPR response associated with a large interlayer interaction which is caused by the structure of nanoflakes and layer edges reached by oxygen. The GNFox and N-GNFox provide the localized and mobile paramagnetic centers which are silent in the pristine (GNF p ) and N-doped (N-GNF) samples. The change in the relative intensity of the line corresponding to delocalized electrons is parallel with the number of radicals in the quaternary N-group. The environment of localized and mobile electrons is different. The results can be important in GNF synthesis and for explanation of their features in applications, especially, in devices with high sensitivity to weak electromagnetic field.