Pre-concentration of short-lived radionuclides using manganese dioxide precipitation from surface waters

Burnett, Jonathan L.; Croudace, Ian W.; Warwick, Phillip E.

doi:10.1007/s10967-011-1392-4

Cited by 12 publications

(7 citation statements)

References 33 publications

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“…Manganese dioxide is used often to preconcentrate Ra for radiochemical analysis. − However, we hypothesized the divalent-rich matrix of FBW would hinder the efficiency of the approach. To test this assertion, we performed MnO 2 preconcentration of FBW to determine if 226 Ra would sorb to MnO 2 or remain in solution.…”

Section: Resultsmentioning

confidence: 99%

“…The method of preconcentration of Ra on MnO 2 has been used often for effective Ra isotopic analysis of water samples. − For our evaluation, 30 mg of KMnO 4 was added to 250 mL of acidified FBW and the pH was adjusted to 7–8 with 6 M ammonium hydroxide (NH 4 OH) to form MnO 2 . Precipitates were filtered on 0.45 μm cellulose nitrate filters (Whatman).…”

Section: Methodsmentioning

confidence: 99%

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Matrix Complications in the Determination of Radium Levels in Hydraulic Fracturing Flowback Water from Marcellus Shale

Nelson

May

Knight

et al. 2014

Environ. Sci. Technol. Lett.

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The rapid proliferation of horizontal drilling and hydraulic fracturing for natural gas mining has raised concerns about the potential for adverse environmental impacts. One specific concern is the radioactivity content of associated "flowback" wastewater (FBW), which is enhanced with respect to naturally occurring radium (Ra) isotopes. Thus, development and validation of effective methods for analysis of Ra in FBW are critical to appropriate regulatory and safety decision making. Recent government documents have suggested the use of EPA method 903.0 for isotopic Ra determinations. This method has been used effectively to determine Ra levels in drinking water for decades. However, analysis of FBW by this method is questionable because of the remarkably high ionic strength and dissolved solid content observed, particularly in FBW from the Marcellus Shale region. These observations led us to investigate the utility of several common Ra analysis methods using a representative Marcellus Shale FBW sample. Methods examined included wet chemical approaches, such as EPA method 903.0, manganese dioxide (MnO 2 ) preconcentration, and 3M Empore RAD radium disks, and direct measurement techniques such as radon (Rn) emanation and high-purity germanium (HPGe) gamma spectroscopy. Nondestructive HPGe and emanation techniques were effective in determining Ra levels, while wet chemical techniques recovered as little as 1% of 226 Ra in the FBW sample studied. Our results question the reliability of wet chemical techniques for the determination of Ra content in Marcellus Shale FBW (because of the remarkably high ionic strength) and suggest that nondestructive approaches are most appropriate for these analyses. For FBW samples with a very high Ra content, large dilutions may allow the use of wet chemical techniques, but detection limit objectives must be considered.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Matrix Complications in the Determination of Radium Levels in Hydraulic Fracturing Flowback Water from Marcellus Shale

Nelson

May

Knight

et al. 2014

Environ. Sci. Technol. Lett.

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“…Samples were spiked with 150–500 mBq of 209 Po, 230 Th, 232 U, and nat U. After appropriate tracers were added, MnO 2 coprecipitations were performed, based on published methods ( Burnett et al 2012 ; Moore 1976 ; Nour et al 2004 ). Potassium permanganate (15 or 30 mg) and bromocresol purple (1 mL, 0.1%) were added to acidified (pH < 2) produced fluid (0.5 L) in glass beakers.…”

Section: Methodsmentioning

confidence: 99%

Understanding the Radioactive Ingrowth and Decay of Naturally Occurring Radioactive Materials in the Environment: An Analysis of Produced Fluids from the Marcellus Shale

Nelson

Eitrheim

Knight

et al. 2015

Environ Health Perspect

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BackgroundThe economic value of unconventional natural gas resources has stimulated rapid globalization of horizontal drilling and hydraulic fracturing. However, natural radioactivity found in the large volumes of “produced fluids” generated by these technologies is emerging as an international environmental health concern. Current assessments of the radioactivity concentration in liquid wastes focus on a single element—radium. However, the use of radium alone to predict radioactivity concentrations can greatly underestimate total levels.ObjectiveWe investigated the contribution to radioactivity concentrations from naturally occurring radioactive materials (NORM), including uranium, thorium, actinium, radium, lead, bismuth, and polonium isotopes, to the total radioactivity of hydraulic fracturing wastes.MethodsFor this study we used established methods and developed new methods designed to quantitate NORM of public health concern that may be enriched in complex brines from hydraulic fracturing wastes. Specifically, we examined the use of high-purity germanium gamma spectrometry and isotope dilution alpha spectrometry to quantitate NORM.ResultsWe observed that radium decay products were initially absent from produced fluids due to differences in solubility. However, in systems closed to the release of gaseous radon, our model predicted that decay products will begin to ingrow immediately and (under these closed-system conditions) can contribute to an increase in the total radioactivity for more than 100 years.ConclusionsAccurate predictions of radioactivity concentrations are critical for estimating doses to potentially exposed individuals and the surrounding environment. These predictions must include an understanding of the geochemistry, decay properties, and ingrowth kinetics of radium and its decay product radionuclides.CitationNelson AW, Eitrheim ES, Knight AW, May D, Mehrhoff MA, Shannon R, Litman R, Burnett WC, Forbes TZ, Schultz MK. 2015. Understanding the radioactive ingrowth and decay of naturally occurring radioactive materials in the environment: an analysis of produced fluids from the Marcellus Shale. Environ Health Perspect 123:689–696; http://dx.doi.org/10.1289/ehp.1408855

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“…Another metal oxide, manganese dioxide (MnO 2 ), has been used to extract a range of toxic elements 3,24,25 and radionuclides 26–29 (particularly radium 30–34 ) from aqueous media for decades. Its use spans the fields of analytical chemistry and drinking water, waste water, and mine water treatment.…”

Section: Introductionmentioning

confidence: 99%

Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions

et al. 2016

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Magnetic nanoparticles are well known to possess chemically active surfaces and large surface areas that can be employed to extract a range of ions from aqueous solutions. Additionally, their superparamagnetic properties provide a convenient means for bulk collection of the material from solution after the targeted ions have been adsorbed. Herein, two nanoscale amphoteric metal oxides, each possessing useful magnetic attributes, were evaluated for their ability to collect trace levels of a chemically diverse range of alpha emitting radioactive isotopes (polonium (Po), radium (Ra), uranium (U), and americium (Am)) from a wide range of aqueous solutions. The nanomaterials include commercially available magnetite (Fe3O4) and magnetite modified to incorporate manganese (Mn) into the crystal structure. The chemical stability of these nanomaterials was evaluated in Hanford Site, WA ground water between the natural pH (~8) and pH 1. Whereas the magnetite was observed to have good stability over the pH range, the Mn-doped material was observed to leach Mn at low pH. The materials were evaluated in parallel to characterize their uptake performance of the alpha-emitting radionuclide spikes from ground water across a range of pH (from ~8 down to 2). In addition, radiotracer uptake experiments were performed on Columbia River water, seawater, and human urine at their natural pH and at pH 2. Despite the observed leaching of Mn from the Mn-doped nanomaterial in the lower pH range, it exhibited generally superior analyte extraction performance compared to the magnetite, and analyte uptake was observed across a broader pH range. We show that the uptake behavior of the various radiotracers on these two materials at different pH levels can generally be explained by the amphoteric nature of the nanoparticle surfaces. Finally, the rate of sorption of the radiotracers on the two materials in unacidified ground water was evaluated. The uptake curves generally indicate that equilibrium is obtained within a few minutes, which is attributed to the high surface areas of the nanomaterials and the high level of dispersion in the liquids. Overall, the results indicate that these nanomaterials may have the potential to be employed for a range of applications to extract radionuclides from aqueous solutions.

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Pre-concentration of short-lived radionuclides using manganese dioxide precipitation from surface waters

Cited by 12 publications

References 33 publications

Matrix Complications in the Determination of Radium Levels in Hydraulic Fracturing Flowback Water from Marcellus Shale

Matrix Complications in the Determination of Radium Levels in Hydraulic Fracturing Flowback Water from Marcellus Shale

Understanding the Radioactive Ingrowth and Decay of Naturally Occurring Radioactive Materials in the Environment: An Analysis of Produced Fluids from the Marcellus Shale

Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions

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