Three-dimensional graphene/titanium dioxide composite for enhanced U(VI) capture: Insights from batch experiments, XPS spectroscopy and DFT calculation

Abstract Efficient containment and capture of uranium (U(VI)) from aqueous solution is an essential component to ensure socially and environmentally sustainable development. Herein, the three-dimensional graphene/titanium dioxide composite (3D GA/TiO2) was synthesized and applied as an effective adsorbent to remove U(VI) from wastewater as a function of contact time, temperature, pH and ion strength. The 3D GA/TiO2 material was characterized by X-ray diffraction, Raman spectroscopy, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The batch experiments results indicated that the adsorption of U(VI) on materials were fitted with the pseudo-second order kinetics and Langmuir models. More specifically, 3D GA/TiO2 (441.3 mg/g) was observed to outperform the GO (280.0 mg/g), rGO (140.9 mg/g) and TiO2 (98.5 mg/g) at pH 5.0, which was attributable to the excellent cooperative effects. Furthermore, XPS analyses and DFT calculations confirmed the formation of surface complexes between oxygen-containing group and U(VI) with the U–O bonds length of 2.348 A (U–O1) and 2.638 A (U–O2). Meanwhile, the adsorption energy was calculated to be 1.60 eV, which showed a very strong chemisorption during the interaction process. It is believed that the 3D GA/TiO2 revealed good removal performance for uranyl ions, which showed a great potential application to control the nuclear industrial pollution.