Abstract
The processes of acid in situ leaching (ISL) uranium (U) mines cause the pollution of groundwater. Phosphate (PO43−) has the potential to immobilize U in groundwater through forming highly insoluble phosphate minerals, but the performance is highly restricted by low pH and high sulfate concentration. In this study, hydrogen peroxide (H2O2) and PO43− were synergistically used for immobilizing U based on the specific properties of groundwater from a decommissioned acid ISL U mine. The removal mechanisms of U and the stability of U on the formed minerals were elucidated by employing X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and kinetic experiments. Our results indicated that the removal of U by simultaneously adding H2O2 and PO43− was significantly higher than the removal of U by individually adding H2O2 or PO43−. The removal of U increased with increasing PO43− concentration from 20 to 200 mg L−1 while decreased with increasing H2O2 concentration from 0.003 to 0.3%. Specifically, the removal efficiency of U from groundwater reached 98% after the application of 0.003% H2O2 and 200 mg L−1 PO43−. Amorphous iron phosphate that preferentially formed at low H2O2 and high PO43− concentrations played a dominant role in U removal, while the formations of schwertmannite and crystalline iron phosphates may be also contributed to the removal of U. This was significantly different from the immobilization mechanism of U through the formation of uranyl phosphate minerals after adding phosphate. The kinetic experimental results suggested that the immobilized U had a good stability. Our research may provide a promising method for in situ remediating U-contaminated groundwater at the decommissioned acid ISL U mines.
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Funding
This study was supported by the National Natural Science Foundation of China (42207309, U1967210), the Natural Science Foundation of Hunan Province (2022JJ40369) and the University of South China Innovation Foundation (X202210555234).
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This study was conceptualized by Y.D. Data collection and analysis were performed by F. L. and Y.D. The experiments were conducted by S.S.W. The first draft of the manuscript was written by F.L. The reviewing and editing of the manuscript were performed by X.X.H., H.Z., J.H.M., Y.D. and D.X.D. The final version of the manuscript has been read and approved by all authors.
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Li, F., Huang, X., Wang, S. et al. Synergistic effects of hydrogen peroxide and phosphate on uranium(VI) immobilization: implications for the remediation of groundwater at decommissioned in situ leaching uranium mine. Environ Sci Pollut Res 30, 117132–117142 (2023). https://doi.org/10.1007/s11356-023-30468-x
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DOI: https://doi.org/10.1007/s11356-023-30468-x