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 »
- Authors:
-
- 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. https://doi.org/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. https://doi.org/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},
url = {https://www.osti.gov/biblio/1330719},
journal = {RSC Advances},
issn = {2046-2069},
number = 107,
volume = 6,
place = {United States},
year = {2016},
month = {10}
}
Web of Science
Works referenced in this record:
Bare magnetic nanoparticles: sustainable synthesis and applications in catalytic organic transformations
journal, January 2014
- Hudson, Reuben; Feng, Yuting; Varma, Rajender S.
- Green Chem., Vol. 16, Issue 10
Functionalized magnetic mesoporous silica nanoparticles for U removal from low and high pH groundwater
journal, November 2016
- Li, Dien; Egodawatte, Shani; Kaplan, Daniel I.
- Journal of Hazardous Materials, Vol. 317
Pre-concentration of short-lived radionuclides using manganese dioxide precipitation from surface waters
journal, August 2011
- Burnett, J. L.; Croudace, I. W.; Warwick, P. E.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 292, Issue 1
Chelate-free metal ion binding and heat-induced radiolabeling of iron oxide nanoparticles
journal, January 2015
- Boros, Eszter; Bowen, Alice M.; Josephson, Lee
- Chemical Science, Vol. 6, Issue 1
Cobalt- and manganese-substituted ferrites as efficient single-site heterogeneous catalysts for aerobic oxidation of monoterpenic alkenes under solvent-free conditions
journal, March 2008
- Menini, L.; Pereira, M.; Parreira, L.
- Journal of Catalysis, Vol. 254, Issue 2
Magnetic nanoparticle-supported crown ethers
journal, January 2007
- Kawamura, Masato; Sato, Kazuhiko
- Chemical Communications, Issue 32
Investigation of Magnetic Nanoparticles for the Rapid Extraction and Assay of Alpha-Emitting Radionuclides from Urine: Demonstration of a Novel Radiobioassay Method
journal, January 2011
- OʼHara, Matthew J.; Carter, Jennifer C.; MacLellan, Jay A.
- Health Physics, Vol. 101, Issue 2
Magnetic recovery of radium, lead and polonium from seawater samples after preconcentration on a magnetic adsorbent of manganese dioxide coated magnetite
journal, July 1996
- Towler, Philip H.; Smith, J. David; Dixon, David R.
- Analytica Chimica Acta, Vol. 328, Issue 1
Polonium-210 and lead-210 in the terrestrial environment: a historical review
journal, May 2011
- Persson, Bertil R. R.; Holm, Elis
- Journal of Environmental Radioactivity, Vol. 102, Issue 5
Magnetite surface charge studies to 290°C from in situ pH titrations
journal, June 2000
- Wesolowski, David J.; Machesky, Michael L.; Palmer, Donald A.
- Chemical Geology, Vol. 167, Issue 1-2
Influence of Calcite and Dissolved Calcium on Uranium(VI) Sorption to a Hanford Subsurface Sediment
journal, October 2005
- Dong, Wenming; Ball, William P.; Liu, Chongxuan
- Environmental Science & Technology, Vol. 39, Issue 20
Synthesis of Highly Selective Magnetic Mesoporous Adsorbent
journal, May 2009
- Chen, Xinqing; Lam, Koon Fung; Zhang, Qingjian
- The Journal of Physical Chemistry C, Vol. 113, Issue 22
Polymer-coated magnetic nanoparticles for rapid bioassay of 90Sr in human urine samples
journal, January 2012
- Varve, Zack; Lai, Edward P. C.; Li, Chunsheng
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 292, Issue 3
Manganese Doping of Magnetic Iron Oxide Nanoparticles: Tailoring Surface Reactivity for a Regenerable Heavy Metal Sorbent
journal, February 2012
- Warner, Cynthia L.; Chouyyok, Wilaiwan; Mackie, Katherine E.
- Langmuir, Vol. 28, Issue 8
Synthesis and ion Exchange Properties of Manganese(Iv) Dioxide Doped by 3+ Transition Metal Cations
journal, May 2001
- Bartoś, Barbara; Bilewicz, Aleksander
- Solvent Extraction and Ion Exchange, Vol. 19, Issue 3
Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model
journal, September 1985
- Hsi, Ching-kuo Daniel; Langmuir, Donald
- Geochimica et Cosmochimica Acta, Vol. 49, Issue 9, p. 1931-1941
Extraction of radium from natural waters using manganese-impregnated acrylic fibers
journal, December 1973
- Moore, Willard S.; Reid, David F.
- Journal of Geophysical Research, Vol. 78, Issue 36
Pre-concentration of actinoids from waters: a comparison of various sorbents
journal, July 2000
- Koulouris, G.; Slowikowski, B.; Pilviö, R.
- Applied Radiation and Isotopes, Vol. 53, Issue 1-2
Dynamic studies on sorption characteristics of226Ra on manganese dioxide
journal, June 1995
- Koulouris, G.
- Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 193, Issue 2
Modeling of Ion-Exchange Reactions on Metal Oxides with the Frumkin Isotherm. 1. Acid−Base and Charge Characteristics of MnO 2 , TiO 2 , Fe 3 O 4 , and Al 2 O 3 Surfaces and Adsorption Affinity of Alkali Metal Ions
journal, January 1996
- Tamura, Hiroki; Katayama, Noriaki; Furuichi, Ryusaburo
- Environmental Science & Technology, Vol. 30, Issue 4
Sorption of Am(III) onto 6-Line-Ferrihydrite and Its Alteration Products: Investigations by EXAFS
journal, June 2006
- Stumpf, Silvia; Stumpf, Thorsten; Dardenne, Kathy
- Environmental Science & Technology, Vol. 40, Issue 11
Application of magnetic nanoparticles for the extraction of radium-226 from water samples
journal, July 2013
- Mesnic, Natalie; Sadi, Baki; Li, Chunsheng
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 3
Removal of heavy metal ions from aqueous solution using Fe3O4–SiO2-poly(1,2-diaminobenzene) core–shell sub-micron particles
journal, December 2012
- Zhang, Fan; Lan, Jing; Zhao, Zongshan
- Journal of Colloid and Interface Science, Vol. 387, Issue 1
Synthesis of amidoxime-functionalized Fe3O4@SiO2 core–shell magnetic microspheres for highly efficient sorption of U(VI)
journal, January 2014
- Zhao, Yingguo; Li, Jiaxing; Zhao, Lanping
- Chemical Engineering Journal, Vol. 235
Solvent extraction study on the hydrolysis of tracer concentration of Po(IV) in chloride solutions
journal, January 1981
- Suganuma, Hideo; Hataye, Itsuhachiro
- Journal of Inorganic and Nuclear Chemistry, Vol. 43, Issue 10
Cation sorption on colloidal hydrous manganese dioxide
journal, December 1968
- Posselt, Hans S.; Anderson, Frederick J.; Weber, Walter J.
- Environmental Science & Technology, Vol. 2, Issue 12
Adsorption characteristics of 210Pb, 210Po and 7Be onto micro-particle surfaces and the effects of macromolecular organic compounds
journal, April 2013
- Yang, Weifeng; Guo, Laodong; Chuang, Chia-Ying
- Geochimica et Cosmochimica Acta, Vol. 107
The point of zero charge of manganese dioxides
journal, May 1978
- Gray, M. J.; Malati, M. A.; rophael, M. W.
- Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 89, Issue 1
The Isoelectric Points of Solid Oxides, Solid Hydroxides, and Aqueous Hydroxo Complex Systems
journal, April 1965
- Parks, George A.
- Chemical Reviews, Vol. 65, Issue 2
Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry
journal, January 1995
- Clark, David L.; Hobart, David E.; Neu, Mary P.
- Chemical Reviews, Vol. 95, Issue 1
EURADOS intercomparison on emergency radiobioassay
journal, December 2014
- Li, Chunsheng; Battisti, Paolo; Berard, Philippe
- Radiation Protection Dosimetry, Vol. 167, Issue 4
Preparation of catalysts by metallic complex adsorption on mineral oxides
journal, January 1978
- Brunelle, J. P.
- Pure and Applied Chemistry, Vol. 50, Issue 9-10
Effect of Crystallographic Structure of MnO 2 on Its Electrochemical Capacitance Properties
journal, February 2008
- Devaraj, S.; Munichandraiah, N.
- The Journal of Physical Chemistry C, Vol. 112, Issue 11
Chemical Insight into the Adsorption of Chromium(III) on Iron Oxide/Mesoporous Silica Nanocomposites
journal, July 2015
- Egodawatte, Shani; Datt, Ashish; Burns, Eric A.
- Langmuir, Vol. 31, Issue 27
Soluble and particle-bound 234,238U, 226Ra and 210Po in ground waters
journal, January 2003
- Vaaramaa, K.; Lehto, J.; Ervanne, H.
- Radiochimica Acta, Vol. 91, Issue 1
First-principles molecular dynamics simulation of the Ca 2 UO 2 (CO 3 ) 3 complex in water
journal, January 2016
- Priest, Chad; Tian, Ziqi; Jiang, De-en
- Dalton Transactions, Vol. 45, Issue 24
Modelling americium sorption onto colloids: effect of redox potential
journal, April 2003
- Alonso, U.; Degueldre, C.
- Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 217, Issue 1-3
Sorption of uranium on magnetite nanoparticles
journal, May 2010
- Das, Debasish; Sureshkumar, M. K.; Koley, Siddhartha
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 285, Issue 3
Determination of the Formation Constants of Ternary Complexes of Uranyl and Carbonate with Alkaline Earth Metals (Mg 2+ , Ca 2+ , Sr 2+ , and Ba 2+ ) Using Anion Exchange Method
journal, August 2006
- Dong, Wenming; Brooks, Scott C.
- Environmental Science & Technology, Vol. 40, Issue 15
The surface chemistry of hydrous manganese dioxide
journal, March 1974
- Murray, James W.
- Journal of Colloid and Interface Science, Vol. 46, Issue 3
Magnetic solids in analytical chemistry: A review
journal, August 2010
- Aguilar-Arteaga, K.; Rodriguez, J. A.; Barrado, E.
- Analytica Chimica Acta, Vol. 674, Issue 2
Selective extraction of 90Sr in urine using 4′4″(5″)di-tert-butyl dicyclohexano-18-crown-6 ether immobilized on polyacrylamide-coated magnetic nanoparticles
journal, September 2014
- Varve, Zack; Lai, Edward P. C.; Li, Chunsheng
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 303, Issue 1
The Sorption of 210Pb, 210Bi and 210Po on Montmorillonite: A Study with Emphasis on Reversibility Aspects and on the Effect of the Radioactive Decay of Adsorbed Nuclides
journal, January 1993
- Ulrich, H. J.; Degueldre, C.
- Radiochimica Acta, Vol. 62, Issue 1-2
Preparation and characterization of manganese dioxide impregnated resin for radionuclide pre-concentration
journal, October 2007
- Varga, Zsolt
- Applied Radiation and Isotopes, Vol. 65, Issue 10
Soluble and Particle-Bound and 210Po 210Pb in Groundwaters
journal, January 1999
- Lehto, J.; Kelokaski, P.; Vaaramaa, K.
- Radiochimica Acta, Vol. 85, Issue 3-4
Identification and characterization of sorbed lutetium species on 2-line ferrihydrite by sorption data modeling, TRLFS and EXAFS
journal, January 2001
- Dardenne, K.; Schäfer, T.; Denecke, Melissa A.
- Radiochimica Acta, Vol. 89, Issue 7
Nanostructured Metal Oxide Sorbents for the Collection and Recovery of Uranium from Seawater
journal, December 2015
- Chouyyok, Wilaiwan; Warner, Cynthia L.; Mackie, Katherine E.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Functionalized Magnetite Nanoparticles—Synthesis, Properties, and Bio-Applications
journal, December 2007
- Majewski, Peter; Thierry, Benjamin
- Critical Reviews in Solid State and Materials Sciences, Vol. 32, Issue 3-4
A surface structural model for ferrihydrite II: Adsorption of uranyl and carbonate
journal, August 2009
- Hiemstra, Tjisse; Riemsdijk, Willem H. Van; Rossberg, André
- Geochimica et Cosmochimica Acta, Vol. 73, Issue 15
Preconcentration of radium isotopes from natural waters using MnO2 Resin
journal, October 2003
- Moon, D. S.; Burnett, W. C.; Nour, S.
- Applied Radiation and Isotopes, Vol. 59, Issue 4
Uranium speciation in waters of different uranium mining areas
journal, June 1998
- Bernhard, G.; Geipel, G.; Brendler, V.
- Journal of Alloys and Compounds, Vol. 271-273
Removal of arsenic from groundwater using low cost ferruginous manganese ore
journal, February 2002
- Chakravarty, S.; Dureja, V.; Bhattacharyya, G.
- Water Research, Vol. 36, Issue 3, p. 625-632
Mineral–Water Interface Reactions of Actinides
journal, October 2012
- Geckeis, Horst; Lützenkirchen, Johannes; Polly, Robert
- Chemical Reviews, Vol. 113, Issue 2
Heavy metal removal from water/wastewater by nanosized metal oxides: A review
journal, April 2012
- Hua, Ming; Zhang, Shujuan; Pan, Bingcai
- Journal of Hazardous Materials, Vol. 211-212
The point of zero charge and adsorption properties of natural magnetite
journal, March 1983
- Milonjić, S. K.; Kopečni, M. M.; Ilić, Z. E.
- Journal of Radioanalytical Chemistry, Vol. 78, Issue 1
Actinide speciation in aquatic systems
journal, March 2006
- Choppin, Gregory R.
- Marine Chemistry, Vol. 99, Issue 1-4
The behavior of scavenged isotopes in marine anoxic environments: 210Pb and 210Po in the water column of the Black Sea
journal, April 1994
- Wei, Ching-Ling; Murray, James W.
- Geochimica et Cosmochimica Acta, Vol. 58, Issue 7
Environmental actinide chemistry
journal, April 1984
- Allard, B.; Olofsson, U.; Torstenfelt, B.
- Inorganica Chimica Acta, Vol. 94, Issue 4
Sorption of 241Am onto Montmorillonite, Illite and Hematite Colloids
journal, January 1994
- Degueldre, C.; Ulrich, H. J. .; Silby, H.
- Radiochimica Acta, Vol. 65, Issue 3
Imaging in Clinical Oncology
journal, February 2015
- Kim, E. E.
- Journal of Nuclear Medicine, Vol. 56, Issue 4
�ber die ?fraktionierte Adsorption? und ?fraktionierte Desadsorption? von Radium-Bariumsalzen and kolloidalem Mangansuperoxydhydrat
journal, November 1913
- Ebler, E.; Bender, W.
- Zeitschrift f�r anorganische Chemie, Vol. 84, Issue 1
International Workshop on Emergency Radiobioassay: Considerations, gaps and Recommendations
journal, January 2011
- Li, Chunsheng; Inn, Kenneth G. W.; Jones, Robert
- Health Physics, Vol. 101, Issue 2
Conjugates of Magnetic Nanoparticle—Actinide Specific Chelator for Radioactive Waste Separation
journal, October 2013
- Kaur, Maninder; Zhang, Huijin; Martin, Leigh
- Environmental Science & Technology, Vol. 47, Issue 21
Removing Radium by Adding Preformed Hydrous Manganese Oxides
journal, February 1990
- Valentine, Richard L.; Spangler, Karen M.; Meyer, John
- Journal - American Water Works Association, Vol. 82, Issue 2
Works referencing / citing this record:
Transforming lanthanide and actinide chemistry with nanoparticles
journal, January 2020
- Pallares, Roger M.; Abergel, Rebecca J.
- Nanoscale, Vol. 12, Issue 3