钚在某处置工程屏障水环境中化学形态及影响因素

针对某放射性废物包装容器回填处置工程屏障结构特征,采用岩体裂隙水浸泡工程屏障样品的方式,在对各平衡水样化学成分分析的基础上,利用地球化学模拟软件EQ3/6对钚在回填工程屏障水环境中的存在化学形态进行了模拟计算,得出钚在回填工程屏障水环境中主要以Pu(Ⅳ)价态Pu(OH)5-形式存在,同时水环境中pH值和Eh值的变化皆会影响钚的存在化学形态和价态。     

QUANTIFICATION OF ACTINIDE MIGRATION PATHWAYS AT ROCKY FLATS,COLORADO1

ABSTRACT: Migration of plutonium, americium, and uranium (actinides) in the environment at the Rocky Flats Environmental Technology Site (RFETS) is the subject of ongoing studies to develop effective strategies for cleanup and regulatory closure of the Department of Energy facility. The Actinide Migration Evaluation pathway analysis quantified actinide transport processes to validate a qualitative conceptual model of environmental actinide transport. Major actinide transport mechanisms evaluated include surface water, ground water, airborne, and biological pathways. Relative quantities of actinide movement via different pathways were compared in terms of actinide loads delivered off the RFETS, using a combination of monitoring data, predictive transport models and results from historic RFETS studies. Results indicate air and surface water constitute the dominant transport mechanisms for plutonium and americium. In ground water, shallow alluvial flow is a limited pathway for plutonium and americium because of the low aqueous solubility of these actinides and their tendency to sorb to soil. However, localized flow in shallow alluvium is a more significant pathway for uranium movement, because of the relatively higher solubility of uranium (VI) species, though isotopic ratios indicate much of the uranium is from natural sources. Biological transport of actinides by mammals, birds, fish, and arthropods is small compared to the other pathways.     

钚同位素法示踪中国领海核爆散落物钚的主要来源与迁移途径

使用电感耦合等离子体质谱仪,对东海及冲绳海槽沉积物、南海及邻近海域以及西北太平洋表层水中240Pu/239Pu同位素比值进行了测定,以确定中国领海核爆散落核素钚的主要来源及迁移途径。结果显示:东海及冲绳海槽沉积物中240Pu/239Pu比值分布于0.24~0.31之间,南海及邻近海域以及西北太平洋表层水240Pu/239Pu比值也处于0.22~0.24之间,都明显高于全球大气理论沉降值0.18。根据240Pu/239Pu比值及其在沉积物芯中的分布特征分析,二十世纪50年代早期美国在北太平洋马绍尔群岛进行的核爆实验,被认为是中国领海及其邻近海域除全球大气沉降外的另一重要的钚的来源。模式计算显示,东海及冲绳沉积物中约55%、中国南海及其邻近海域表层水中约40%、西北太平洋表层水中约20%的钚,来自北太平洋核爆基地。北太平洋赤道环流及其在西北太平洋的分支洋流是钚自核爆地向中国领海迁移的主要通道。