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Investigation of in Situ Leach (ISL) Mining of Uranium in New Mexico and Post-Mining Reclamation Omar Ruiz, Bruce M

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Investigation of in Situ Leach (ISL) Mining of Uranium in New Mexico and Post-Mining Reclamation Omar Ruiz, Bruce M Investigation of in situ leach (ISL) mining of uranium in New Mexico and post-mining reclamation Omar Ruiz, Bruce M. Thomson, Jose M. Cerrato Center for Water & the Environment, Department of Civil Engineering, University of New Mexico Abstract peroxide) and a carbonate-complexing agent. It is The purpose of this study was to consider the injected into the aquifer to solubilize U by oxidizing effectiveness of two methods of restoring groundwater it to more soluble phases, which then dissolve through quality in a subsurface uranium-bearing formation a series of complexation reactions. The soluble U following in situ leach (ISL) mining. To accomplish complexes are transported by groundwater flow to the this it was necessary to develop an understanding of extraction wells where they are pumped to the surface the geochemical characteristics of an aqueous solution and are recovered in a mill. The barren lixiviant is then that might be produced by an ISL mine. Samples pumped back into the aquifer through injection wells of material from three different uranium (U) mines and the process is repeated. were collected and their acid leachable elemental The major advantages of ISL mining are that (U.S. concentration determined. Additional samples Nuclear Regulatory Commission, 2009): 1) it produces were then leached with aerated sodium bicarbonate little disturbance of the land surface, 2) construction costs (NaHCO3) solutions at concentrations ranging from 1 mM to 500 mM. The fraction of the acid-leachable are much less than conventional underground mining, 3) U and other trace elements released by this leaching it is much safer for workers than underground mining, 4) very little solid waste is generated because there is process depended on NaHCO3 concentration, U mineralogy, and the amount of solid organic matter virtually no excavation, and 5) there is little impact on in the samples. Less than 5% U was leached from groundwater resources due to mine dewatering. Often samples with high organic matter using the NaHCO3 these advantages result in significant cost savings. leach solution. Groundwater restoration methods However, there are also notable limitations of were then investigated using column experiments. ISL mining. The ore deposit must be below the water Two methods were evaluated, a chemical stabilization table; the hydrogeology of the host formation must be method based on addition of phosphate (PO4) and a microbial method in which lactate was added to amenable to circulation of lixiviant solutions through stimulate growth of dissimilatory sulfate and metal it; and the U minerals must be reactive with the leach reducing organisms. Neither method was effective. solutions. Though ISL mining has been extensively This was believed to be due to sweeping of the leach practiced in other states, there is little experience with solution from the columns by the phosphate- or lactate- it in New Mexico. amended solutions. This hypothesis is consistent with A major challenge facing the ISL mining industry limited mixing in an aquifer as a result of plug flow is that groundwater must be returned to acceptable through the formation. quality at the conclusion of mining. ISL mining alters the geochemistry of the ore body resulting in release Introduction of other constituents at concentrations that may exceed New Mexico has played a major role in the production state groundwater standards and federal drinking of uranium (U) for the nuclear power industry and the water standards. In New Mexico, aquifer restoration is nation’s weapons programs, producing more than 340 M especially important because groundwater may be the lbs of yellowcake (U3O8) (McLemore et al., 2013). Though sole water supply for drinking and other uses, such as the U mining and milling industry in New Mexico is in the Grants Mining District. inactive at present, increased interest in nuclear energy The principal objective of this research was to evaluate as a CO2-free power source has led to renewed interest two methods of stabilizing aqueous geochemistry and in development of U resources. Recently, projects have of restoring groundwater quality following ISL mining. been proposed using both conventional underground A two-phase laboratory investigation was conducted in mining and in situ leach (ISL) mining. which different leach solutions were used to evaluate Currently, nearly all United States U production is extraction of U from several low-grade ore samples. from ISL mines. In 2015, total U.S. production was 3.3 In contrast to other studies, which were done in batch M lbs of U3O8 from one underground mine and six ISL systems, this investigation was performed using columns mines (U.S. Energy Information Administration 2016). filled with U ore to better simulate ISL conditions. The The ISL mines are located in Nebraska, Texas, and purpose was to generate information regarding the Wyoming. Note that the domestic U industry continues chemistry of fluids that would be produced by ISL mining to struggle as reflected by the fact that total production of NM U ores. The second phase of the investigation in 2015 was 32% less than in 2014 (U.S. Energy consisted of a series of column studies to evaluate Information Administration, 2016). two strategies for restoring groundwater quality. One ISL mining, also referred to as in situ recovery method was based on chemical addition to stabilize (ISR) mining, is accomplished by using a system of minerals that release U and other constituents. This injection and extraction wells to circulate a solution or involved circulation of a phosphate (PO4) solution. The “lixiviant,” through the subsurface ore formation (U.S. second method was based on re-establishing reducing Nuclear Regulatory Commission, 2009). The lixiviant conditions in the aquifer by stimulating growth of typically consists of an oxidant (oxygen or hydrogen anaerobic microorganisms. November 2016, Volume 38, Number 4 New Mexico Geology 77 2- Background and theoretical considerations and carbonate (CO3 ) near neutral pH have also been reported (Dong and Brooks 2006), but for the sake This section provides a brief summary of the theoretical of simplicity are not shown on this diagram. Because most considerations associated with ISL U mining in order to soil minerals have net negative surface charges above pH establish a fundamental basis for the research described in ~ 5, uranyl-carbonate complexes do not interact with soil this paper. This summary also includes a brief overview of mineral surfaces and therefore are readily transported ISL mining and previous groundwater restoration studies. by groundwater through aquifer materials. In contrast, Geochemistry of uranium and co-constituents U(IV) forms insoluble precipitates; uraninite (UO2(s)) and coffinite (USiO4(s)) are shown in this diagram. Deep ore In the natural environment, U most commonly occurs deposits often are dominated by reduced U phases of in two oxidation states, U(IV) and U(VI). Uranium which nearly 100 different minerals are known (De Voto, geochemistry strongly depends on its oxidation state 1978; Burns and Finch, 1999). and the presence of inorganic complexants, especially Extracting insoluble U from ore generally involves carbonate (CO ). Its geochemistry can be conveniently 3 oxidation followed by dissolution whether in a conventional summarized in a pe-pH diagram (also referred to as an mill or in an ISL mine (Thomson and Heggen, 1983). In a Eh-pH diagram) in which the oxidation-reduction (redox) conventional mill, ore is pulverized then leached with an conditions of the solution are plotted on the vertical axis oxygenated strong acid such as sulfuric acid or a strong and acid-base conditions are plotted on the horizontal axis basic carbonate solution. The dissolved U is then recovered (Langmuir, 1997). A pe-pH diagram for U is presented from solution by ion exchange (IX) or solvent extraction. in Figure 1. This diagram represents U-equilibrium -6 -3 In an ISL mine an oxygenated carbonate solution is chemistry in a solution containing 10 M U and 10 M circulated through the formation to oxidize, complex and dissolved CO at 25°C. The diagram shows that under 2 dissolve the U, which is then recovered at the surface by oxidizing conditions, U(VI) is thermodynamically stable, IX. The geochemical reactions in the ISL process have and its speciation depends on the pH of the solution. been presented elsewhere (Davis and Curtis, 2007). Below pH 5, the cationic uranyl ion (UO 2+) is present, 2 Several other metals and metalloids have redox while at higher pH the uranyl ion forms soluble mono-, chemistry similar to U, including arsenic (As), molybdenum di-, and tri-carbonate complexes. These complexes are 2+ (Mo), selenium (Se), and vanadium (V). Accordingly, it is soluble. Ternary complexes of uranyl with calcium (Ca ) common to find one or more of these elements present 25 1.4 20 1.2 O 2 H O 2 1.0 15 UO ++ 0.8 2 10 UO (CO )0 0.6 2 3 UO (CO ) 2- 2 3 2 0.4 USiO 5 4 (s) UO (CO ) 4- 2 3 3 0.2 4+ (volts) pE U 0 0 Eh H O 2 UO 2 (s) -0.2 -5 H 2 -0.4 -10 -0.6 -0.8 -15 0 2 4 6 8 10 12 14 pH Figure 1. pe-pH diagram for U for a closed system where the total U concentration is 10-6 M and the total -3 dissolved CO2 and H4SiO4 concentrations are 10 M (diagram prepared by Thomson after Langmuir, 1997). 78 New Mexico Geology November 2016, Volume 38, Number 4 in U-bearing formations or as mixed U minerals such Rock and Crownpoint mines proposed by HydroResources . as carnotite (K2(UO2)2(VO4)2 1-3H2O or tyuyamunite Inc., both with a planned capacity of 1 M lbs/yr of U3O8. (Ca(UO2)2(VO4)2 5-8H2O).
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