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Lawrinenko, M., Kurwadkar, S., & Wilkin, R. T. (2023). Long-term performance evaluation of zero-valent iron amended permeable reactive barriers for groundwater remediation – A mechanistic approach. Geoscience Frontiers, 14(2), 101494.
Abstract: Permeable reactive barriers (PRBs) are used for groundwater remediation at contaminated sites worldwide. This technology has been efficient at appropriate sites for treating organic and inorganic contaminants using zero-valent iron (ZVI) as a reductant and as a reactive material. Continued development of the technology over the years suggests that a robust understanding of PRB performance and the mechanisms involved is still lacking. Conflicting information in the scientific literature downplays the critical role of ZVI corrosion in the remediation of various organic and inorganic pollutants. Additionally, there is a lack of information on how different mechanisms act in tandem to affect ZVI-groundwater systems through time. In this review paper, we describe the underlying mechanisms of PRB performance and remove isolated misconceptions. We discuss the primary mechanisms of ZVI transformation and aging in PRBs and the role of iron corrosion products. We review numerous sites to reinforce our understanding of the interactions between groundwater contaminants and ZVI and the authigenic minerals that form within PRBs. Our findings show that ZVI corrosion products and mineral precipitates play critical roles in the long-term performance of PRBs by influencing the reactivity of ZVI. Pore occlusion by mineral precipitates occurs at the influent side of PRBs and is enhanced by dissolved oxygen and groundwater rich in dissolved solids and high alkalinity, which negatively impacts hydraulic conductivity, allowing contaminants to potentially bypass the treatment zone. Further development of site characterization tools and models is needed to support effective PRB designs for groundwater remediation.
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Hall, S. M., Gosen, B. S. V., Paces, J. B., Zielinski, R. A., & Breit, G. N. (2019). Calcrete uranium deposits in the Southern High Plains, USA. Ore Geology Reviews, 109, 50–78.
Abstract: The Southern High Plains (SHP) is a new and emerging U.S. uranium province. Here, uranyl vanadates form deposits in Pliocene to Pleistocene sandstone, dolomite, and limestone. Fifteen calcrete uranium occurrences are identified; two of these, the Buzzard Draw and Sulfur Springs Draw deposits, have combined in-place resources estimated at about 4 million pounds of U3O8. Ore minerals carnotite and finchite are hosted in dolomite at the Sulfur Springs Draw deposit, with accessory fluorite, celestine, smectite/illite, autunite, and strontium carbonate. Host carbonate at the Sulfur Springs Draw deposit is ∼190 ka and mineralization mobilized as recently as 3.8 ka. Ash collected near the deposit is 631 ka and erupted from the Yellowstone caldera complex. The Triassic Dockum Group that contains sandstone-hosted uranium deposits throughout the region and underlies the SHP is a potential source for uranium and vanadium. Regional uplift and dissection reintroduced oxygenated groundwater into the Dockum Group, mobilizing uranium. Additional uranium may have been contributed to groundwater by weathering of volcanic ash in Pliocene and Pleistocene host rocks. The locations of the uranium occurrences are mostly in modern drainage systems in the southeast portion of the SHP. Modelling of modern groundwater in the SHP carried out in a parallel study shows that a single fluid could form carnotite through evaporation, and that fluids of the requisite composition are more prevalent in the southern portion of the SHP. The southeastern portion of the SHP hosts more uranium occurrences due to a variety of factors including (1) upward transport of groundwater and connectivity between source and host rock, (2) higher uranium and vanadium content of groundwater, (3) higher rates of groundwater recharge in this region to drive the mineralizing system, and (4) shallower groundwater facilitating surface evaporation. Ongoing erosion of host rocks challenges preservation of deposits and may limit their size.
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Milena-Pérez, A., Piñero-García, F., Benavente, J., Expósito-Suárez, V. M., Vacas-Arquero, P., & Ferro-García, M. A. (2021). Uranium content and uranium isotopic disequilibria as a tool to identify hydrogeochemical processes. Journal of Environmental Radioactivity, 227, 106503.
Abstract: This paper studies the uranium content and uranium isotopic disequilibria as a tool to identify hydrogeochemical processes from 52 groundwater samples in the province of Granada (Betic Cordillera, southeastern Spain). According to the geological complexity of the zone, three groups of samples have been considered. In Group 1 (thermal waters; longest residence time), the average uranium content was 2.63 ± 0.16 μg/L, and 234U/238U activity ratios (AR) were the highest of all samples, averaging 1.92 ± 0.30. In Group 2 (mainly springs from carbonate aquifers; intermediate residence time), dissolved uranium presented an average value of 1.34 ± 0.13 μg/L, while AR average value was 1.38 ± 0.25. Group 3 comes from pumping wells in a highly anthropized alluvial aquifer. In this group, where the residence time of the groundwater is the shortest of the three, average uranium content was 5.28 ± 0.26 μg/L, and average AR is the lowest (1.17 ± 0.12). In addition, the high dissolved uranium value and the low AR brought to light the contribution of fertilizers (Group 3). In the three groups, 235U/238U activity ratios were similar to the natural value of 0.046. Therefore, 235U detected in the samples comes from natural sources. This study is completed with the determination of major ions and physicochemical parameters in the groundwater samples and the statistical analysis of the data by using the Principal Component Analysis. This calculation indicates the correlation between uranium isotopes and bicarbonate and nitrate anions.
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