Extremely defect
graphene oxide (dGO) is proposed as an advanced
sorbent for treatment of radioactive waste and contaminated natural
waters. dGO prepared using a modified Hummers oxidation procedure,
starting from reduced graphene oxide (rGO) as a precursor, shows significantly
higher sorption of U(VI), Am(III), and Eu(III) than standard graphene
oxides (GOs). Earlier studies revealed the mechanism of radionuclide
sorption related to defects in GO sheets. Therefore, explosive thermal
exfoliation of graphite oxide was used to prepare rGO with a large
number of defects and holes. Defects and holes are additionally introduced
by Hummers oxidation of rGO, thus providing an extremely defect-rich
material. Analysis of characterization by XPS, TGA, and FTIR shows
that dGO oxygen functionalization is predominantly related to defects,
such as flake edges and edge atoms of holes, whereas standard GO exhibits
oxygen functional groups mostly on the planar surface. The high abundance
of defects in dGO results in a 15-fold increase in sorption capacity
of U(VI) compared to that in standard Hummers GO. The improved sorption
capacity of dGO is related to abundant carboxylic group attached hole
edge atoms of GO flakes as revealed by synchrotron-based extended
X-ray absorption fine structure (EXAFS) and high-energy resolution
fluorescence detected X-ray absorption near edge structure (HERFD-XANES)
spectroscopy.