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

Abstract

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. In addition, their superparamagnetic properties provide a convenient means for bulk collection of the material from solution after the targeted ions have been adsorbed. We evaluated two nanoscale amphoteric metal oxides, each possessing useful magnetic attributes 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,more » 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. In sum, our results indicate that these nanomaterials may have the potential to be employed for a range of applications to extract radionuclides from aqueous solutions.« less

Authors:
 [1];  [1];  [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1330719
Grant/Contract Number:  
AC0576RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 6; Journal Issue: 107; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

O'Hara, Matthew J., Carter, Jennifer C., Warner, Cynthia L., Warner, Marvin G., and Addleman, R. Shane. Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions. United States: N. p., 2016. Web. doi:10.1039/C6RA22262E.
O'Hara, Matthew J., Carter, Jennifer C., Warner, Cynthia L., Warner, Marvin G., & Addleman, R. Shane. Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions. United States. doi:10.1039/C6RA22262E.
O'Hara, Matthew J., Carter, Jennifer C., Warner, Cynthia L., Warner, Marvin G., and Addleman, R. Shane. Mon . "Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions". United States. doi:10.1039/C6RA22262E. https://www.osti.gov/servlets/purl/1330719.
@article{osti_1330719,
title = {Magnetic iron oxide and manganese-doped iron oxide nanoparticles for the collection of alpha-emitting radionuclides from aqueous solutions},
author = {O'Hara, Matthew J. and Carter, Jennifer C. and Warner, Cynthia L. and Warner, Marvin G. and Addleman, R. Shane},
abstractNote = {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. In addition, their superparamagnetic properties provide a convenient means for bulk collection of the material from solution after the targeted ions have been adsorbed. We evaluated two nanoscale amphoteric metal oxides, each possessing useful magnetic attributes 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. In sum, our results indicate that these nanomaterials may have the potential to be employed for a range of applications to extract radionuclides from aqueous solutions.},
doi = {10.1039/C6RA22262E},
journal = {RSC Advances},
number = 107,
volume = 6,
place = {United States},
year = {Mon Oct 31 00:00:00 EDT 2016},
month = {Mon Oct 31 00:00:00 EDT 2016}
}

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Works referenced in this record:

Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model
journal, September 1985


Removal of arsenic from groundwater using low cost ferruginous manganese ore
journal, February 2002