Hu Q H, Rose T P, Zavarin M, Smith D K, Moran J E, Zhao P H
College of Water Sciences, Beijing Normal University, Xinjiekouwai Street 19, Beijing 100875, PR China.
J Environ Radioact. 2008 Oct;99(10):1617-30. doi: 10.1016/j.jenvrad.2008.06.007. Epub 2008 Jul 26.
Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (3H, 14C, 36Cl, 99Tc and 129I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and 36Cl showed little evidence of retardation, while the transport of 14C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially 99Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of 129I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some "mobile" radionuclides (especially 99Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.
由于1951年至1992年间在内华达试验场(NTS)进行了828次地下核武器试验,许多长寿命放射性核素存在于该试验场的地下水中。结合对可能在地下迁移的放射性核素(3H、14C、36Cl、99Tc和129I)进行的全面地球化学审查,我们综合了从18口监测井采集的地下水样本中测得的一系列放射性核素活度数据,以定性评估它们在内华达试验场数百米距离和数十年时间尺度上的迁移情况。氚和36Cl几乎没有显示出滞留的迹象,而14C的迁移可能因其与含水层中碳酸盐矿物的同位素交换而受到阻碍。观测到的局部还原条件(自然的或试验引起的)将影响某些对氧化还原敏感的放射性核素(尤其是99Tc)的迁移性,这些核素在氧化条件下原本是可溶的且易于迁移。相反,强氧化条件可能会影响129I的迁移性,129I在还原条件下是可迁移的。碘的形态对其迁移的影响值得进一步关注。在内华达试验场地下水中一些“可迁移”放射性核素(尤其是99Tc)出现延迟迁移的迹象,表明自然系统的氧化还原条件在控制放射性核素的归宿和迁移方面具有重要意义,这对位于内华达试验场附近的潜在尤卡山核废料储存库增强储存高放核废料的性能以及对遗留核作业设施中的放射性核素污染管理都有影响。