Nehete Sachin Vilas, Christensen Terje, Salbu Brit, Teien Hans-Christian
Centre of Environmental Radioactivity CoE, Department of Environmental Sciences, Norwegian University of Life Sciences (NMBU), P. O. Box 5003, 1432, Ås, Norway.
Centre of Environmental Radioactivity CoE, Norwegian Radiation Protection Authority (NRPA), P. O. Box 55, 1332, Østerås, Norway.
J Chromatogr A. 2017 May 5;1496:105-114. doi: 10.1016/j.chroma.2017.03.042. Epub 2017 Mar 21.
Humic substances have a tendency to form complexes with metal ions in aquatic medium, impacting the metal mobility, decreasing bioavailability and toxicity. Ultraviolet-B (UV-B) radiation exposure degrades the humic substance, changes their molecular weight distribution and their metal binding capacity in aquatic medium. In this study, we experimented the effect of UV-B radiation on the uranium complexed with fulvic acids and humic acids in a soft water system at different pH, uranium concentrations and radiant exposure. The concentration and distribution of uranium in a complexed form were investigated by asymmetrical flow field-flow fractionation coupled to multi detection technique (AsFlFFF-UV-ICP-MS). The major concentration of uranium present in complexes was primarily associated with average and higher molecular weight fulvic and humic acids components. The concentration of uranium in a complexed form increased with increasing fulvic and humic acid concentrations as well as pH of the solution. The higher molecular weight fraction of uranium was degraded due to the UV-B exposure, transforming about 50% of the uranium-dissolved organic carbon complexes into low molecular weight uranium species in complex form with organic ligands and/or free form. The result also suggests AsFlFFF-UV-ICP-MS to be an important separation and detection technique for understanding the interaction of radionuclides with dissolved organic matter, tracking size distribution changes during degradation of organic complexes for understanding mobility, bioavailability and ecosystem transfer of radionuclides as well as metals.
腐殖质在水生介质中倾向于与金属离子形成络合物,影响金属的迁移性,降低生物有效性和毒性。紫外线-B(UV-B)辐射会使腐殖质降解,改变其分子量分布及其在水生介质中的金属结合能力。在本研究中,我们在不同pH值、铀浓度和辐射暴露条件下,在软水体系中试验了UV-B辐射对与富里酸和腐殖酸络合的铀的影响。采用不对称流场-流分馏结合多检测技术(AsFlFFF-UV-ICP-MS)研究了络合态铀的浓度和分布。络合物中铀的主要浓度主要与平均分子量和较高分子量的富里酸和腐殖酸组分相关。络合态铀的浓度随富里酸和腐殖酸浓度以及溶液pH值的增加而增加。由于UV-B辐射,较高分子量的铀组分发生降解,约50%的铀-溶解有机碳络合物转化为与有机配体呈络合形式和/或游离形式的低分子量铀物种。结果还表明,AsFlFFF-UV-ICP-MS是一种重要的分离和检测技术,可用于理解放射性核素与溶解有机物的相互作用,追踪有机络合物降解过程中的粒径分布变化,以了解放射性核素以及金属的迁移性、生物有效性和生态系统转移情况。