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Influences on Subsurface Plutonium and Americium Migration
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2021-02-04 , DOI: 10.1021/acsearthspacechem.0c00277 Hilary P. Emerson 1 , Carolyn I. Pearce 1 , Calvin H. Delegard 2 , Kirk J. Cantrell 1 , Michelle M.V. Snyder 1 , May-Lin Thomas 1 , Brandy N. Gartman 1 , Micah D. Miller 1 , Charles T. Resch 1 , Steve M. Heald 3 , Andrew E. Plymale 1 , Dallas D. Reilly 1 , Sarah A. Saslow 1 , William Neilson 4 , Samuel Murphy 4 , Mavrik Zavarin 5 , Annie B. Kersting 5 , Vicky L. Freedman 1
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2021-02-04 , DOI: 10.1021/acsearthspacechem.0c00277 Hilary P. Emerson 1 , Carolyn I. Pearce 1 , Calvin H. Delegard 2 , Kirk J. Cantrell 1 , Michelle M.V. Snyder 1 , May-Lin Thomas 1 , Brandy N. Gartman 1 , Micah D. Miller 1 , Charles T. Resch 1 , Steve M. Heald 3 , Andrew E. Plymale 1 , Dallas D. Reilly 1 , Sarah A. Saslow 1 , William Neilson 4 , Samuel Murphy 4 , Mavrik Zavarin 5 , Annie B. Kersting 5 , Vicky L. Freedman 1
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Plutonium (Pu) has been released to the environment worldwide, including approximately 1.85 × 1015 Bq (200 kg) of Pu from process waste solutions to unconfined soil structures at the Hanford Site in Washington State. The subsurface mobility of Pu is influenced by complex interactions with sediments, groundwater, and any co-contaminants within the waste stream. Previous investigations at Hanford have shown that Pu exists as discrete PuO2 particles forming before or after disposal, as secondary solid phases formed from waste interactions with sediments as adsorbed/incorporated species, and/or as dissolved species. In this research, new evidence is presented for the existence of PuO2, PuO2-Bi2O3 composites, and particles from burnt Pu metal in near-surface sediments where Pu-laden acidic process waste was disposed to sediments. Pu and americium (Am) L3 X-ray absorption spectroscopy and density functional theory suggest that, in larger, more crystalline PuO2 particles, Am formed from radioactive decay is retained in the PuIVO2 structure as AmIV. The Pu and Am that were disposed of in an acidic waste stream have since migrated deeper into the subsurface with detection to at least 37 meters below ground surface. In contrast, Pu deposited near the ground surface from neutral pH waste is found to be homogeneously distributed and relatively immobile. Groundwater extractions performed on contaminated sediments indicate that both Pu and Am are recalcitrant, with Am being fractionally less extractable than Pu on a molar basis. These results suggest that the more mobile fraction of Am has migrated from the near-surface and may be present in the deeper sediments as a different phase than Pu. From these results, it is suggested that Pu and Am deposited from acidic wastes were initially mobile and became significantly less mobile as wastes were neutralized within the soil profile.
中文翻译：
对地下P和Migration迁移的影响
Washington（Pu）已释放到全世界的环境中，其中约有1.85×10 15 Bq（200 kg）的Pu从过程废液到华盛顿州汉福德工厂的无限制土壤结构。Pu的地下流动性受与沉积物，地下水和废物流中任何共污染物的复杂相互作用的影响。汉福德（Hanford）的先前研究表明，Pu以离散的PuO 2颗粒的形式存在，在处置之前或之后形成，次生固相是由废物与沉积物（作为吸附/结合物种和/或溶解物种）相互作用而形成的次级固相。在这项研究中，为存在PuO 2，PuO 2 -Bi 2 O 3提供了新的证据。复合材料，以及来自近地表沉积物中燃烧的Pu金属的颗粒，在其中沉积了含Pu酸性工艺废料。Pu和a（Am）L 3 X射线吸收光谱法和密度泛函理论表明，在更大，更结晶的PuO 2颗粒中，由放射性衰变形成的Am与Am IV一样保留在Pu IV O 2结构中。自那时以来，被处置在酸性废物流中的Pu和Am迁移至更深的地下，并被发现到地下至少37米。相反，发现中性pH废物在地面附近沉积的Pu分布均匀且相对不动。在受污染的沉积物上进行的地下水提取表明，Pu和Am都是难降解的，以摩尔计，Am的可提取性比Pu低。这些结果表明，流动性较高的Am组分已从近地表迁移出来，并可能以与Pu不同的相存在于较深的沉积物中。从这些结果可以看出，酸性废物中沉积的Pu和Am最初是可移动的，随着废物在土壤剖面中被中和，其流动性大大降低。
更新日期：2021-02-18
中文翻译：
对地下P和Migration迁移的影响
Washington（Pu）已释放到全世界的环境中，其中约有1.85×10 15 Bq（200 kg）的Pu从过程废液到华盛顿州汉福德工厂的无限制土壤结构。Pu的地下流动性受与沉积物，地下水和废物流中任何共污染物的复杂相互作用的影响。汉福德（Hanford）的先前研究表明，Pu以离散的PuO 2颗粒的形式存在，在处置之前或之后形成，次生固相是由废物与沉积物（作为吸附/结合物种和/或溶解物种）相互作用而形成的次级固相。在这项研究中，为存在PuO 2，PuO 2 -Bi 2 O 3提供了新的证据。复合材料，以及来自近地表沉积物中燃烧的Pu金属的颗粒，在其中沉积了含Pu酸性工艺废料。Pu和a（Am）L 3 X射线吸收光谱法和密度泛函理论表明，在更大，更结晶的PuO 2颗粒中，由放射性衰变形成的Am与Am IV一样保留在Pu IV O 2结构中。自那时以来，被处置在酸性废物流中的Pu和Am迁移至更深的地下，并被发现到地下至少37米。相反，发现中性pH废物在地面附近沉积的Pu分布均匀且相对不动。在受污染的沉积物上进行的地下水提取表明，Pu和Am都是难降解的，以摩尔计，Am的可提取性比Pu低。这些结果表明，流动性较高的Am组分已从近地表迁移出来，并可能以与Pu不同的相存在于较深的沉积物中。从这些结果可以看出，酸性废物中沉积的Pu和Am最初是可移动的，随着废物在土壤剖面中被中和，其流动性大大降低。
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