Abstract
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•Sulfonated graphene oxide (SGO) was synthesized successfully.•The SGO had high sorption capacity of U(VI) at ultralow pH.•The interaction of U(VI) with SGO was characterized by XPS, EXAFS and DFT.•The sulfonyl groups contributed U(VI) interaction at low pH.•U(VI) sorption was attributed to oxygen-containing functional groups at high pH.
The interaction mechanism of high effective enrichment of U(VI) on sulfonated graphene oxide (GO) at ultralow pH still remains unclear. The batch characteristic results showed that sulfonated GO presented a variety of functional groups such as hydroxyl (OH), carboxyl (COOH) and sulfonyl (OSO3H) groups. The macroscopic results indicated that the sorption of U(VI) on sulfonated GO was independent of ionic strength, and the maximum sorption capacity calculated from Langmuir model was 45.05mg/g at pH 2.0. The change of relative intensities for S 2p spectra was significantly higher than that of O 1s spectra by XPS analysis. According to EXAFS analysis, the significant splitting of equatorial oxygen (U-Oeq) shell at pH 2.0 was attributed to the electron scattering of the elemental sulfur. The energy of uranyl-sulfonyl (−3198.511hartree/particle) at pH 2.0 calculated based on theoretical calculations was lower than that of uranyl-carboxyl (−3198.498hartree/particle), indicating that uranyl-sulfonyl was more stable at ultralow pH. These observations indicated that the sulfonyl of GO was responsible for high effective removal of U(VI) at ultralow pH, which is vital to the application of functionalized GO in the preconcentration of U(VI) in nuclear waste management and the removal of U(VI) from wastewater at low pH values.