Abstract:
A considerable amount of waste solution of low uranium concentration is generated during the fuel production for high-temperature gas-cooled reactors, it contains high concentration of urea and some organics including polyvinyl and tetrahydrofurfuryl alcohol. In order to remove uranium from the low-level wastewate using TiO
2/Ti electrochemical method, the electrode was prepared by annealing Ti flakes at 680 ℃ for 2 h, the effect on uranium removal efficiency of varying parameters, such as the concentration of sodium carbonate, pH of the solution, time, the concentration of uranium, and voltage of the working electrode, and the mechanism for removing uranium was proposed. The results from scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffractometer (XRD) indicate that a layer of nanoscale oxide particles is formed on the surface of the TiO
2/Ti electrode during the annealing treatment. Under optimized conditions, over 95.43% of uranium can be removed from the solution of 0.01 mol/L sodium carbonate within 5 h under electrode voltage of 10 V. Cyclic voltammetry tests show that only one pair of redox peaks for uranium at −0.99 V and −0.48 V (vs SCE) exist in the potential range of −2 V to 0.5 V (vs SCE), and square wave voltammetry tests show that only one electron transfer involves in the process of uranium deposition on the electrode, indicating that the reduction process of uranium is going through two steps, first U(Ⅵ) gets an electron to be reduced to U(Ⅴ) controlled by diffusion, then U(Ⅴ) disproportionates to U(Ⅳ) and U(Ⅵ). The results of reduction product characterization show that uranium is deposited on the electrode surface in the form of mixed UO
2 and U
2O
5. The experimental results of uranium removal show that the electrodeposition rate of uranium gradually slows down after 5 h. With additional working time, for example, at 10 h, the removal rate of uranium can reach 98.52%. Uranium removal rate is above 90% in the solution pH=3-11 range and in the initial uranium concentration range of 10-500 mg/L. Among the organic substances, urea and polyvinyl significantly inhibit uranium removal, while tetrahydrofurfuryl alcohol does not. In addition, uranium removal rate decreases rapidly with increasing ammonium nitrate concentration.