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

O'Hara, Matthew J.; Carter, Jennifer C.; Warner, Cynthia L.; Warner, Marvin G.; Addleman, R. Shane

doi:10.1039/C6RA22262E

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

Journal Article · Mon Oct 31 00:00:00 EDT 2016 · RSC Advances

DOI:https://doi.org/10.1039/C6RA22262E· OSTI ID:1330719

O'Hara, Matthew J. ^[1]; Carter, Jennifer C. ^[1]; Warner, Cynthia L. ^[1]; Warner, Marvin G. ^[1]; Addleman, R. Shane ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1330719

Alternate ID(s):: OSTI ID: 1339852

Journal Information:: RSC Advances, Journal Name: RSC Advances Journal Issue: 107 Vol. 6; ISSN 2046-2069; ISSN RSCACL

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (69)

Magnetic Nanomaterials for Environmental Applications Warner, Marvin G.; Warner, Cynthia L.; Addleman, R. Shane Nanotechnologies for the Life Sciences: Online https://doi.org/10.1002/9783527610419.ntls0171	book	September 2007
Removing Radium by Adding Preformed Hydrous Manganese Oxides Valentine, Richard L.; Spangler, Karen M.; Meyer, John Journal - American Water Works Association, Vol. 82, Issue 2 https://doi.org/10.1002/j.1551-8833.1990.tb06921.x	journal	February 1990
�ber die ?fraktionierte Adsorption? und ?fraktionierte Desadsorption? von Radium-Bariumsalzen and kolloidalem Mangansuperoxydhydrat Ebler, E.; Bender, W. Zeitschrift f�r anorganische Chemie, Vol. 84, Issue 1 https://doi.org/10.1002/zaac.19130840106	journal	November 1913
Imaging in Clinical Oncology Gouliamos, Athanasios D.; Andreou, John; Kosmidis, Paris https://doi.org/10.1007/978-88-470-5385-4	book	January 2014
Dynamic studies on sorption characteristics of226Ra on manganese dioxide Koulouris, G. Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 193, Issue 2 https://doi.org/10.1007/BF02039884	journal	June 1995
The point of zero charge and adsorption properties of natural magnetite Milonjić, S. K.; Kopečni, M. M.; Ilić, Z. E. Journal of Radioanalytical Chemistry, Vol. 78, Issue 1 https://doi.org/10.1007/BF02519745	journal	March 1983
Sorption of uranium on magnetite nanoparticles Das, Debasish; Sureshkumar, M. K.; Koley, Siddhartha Journal of Radioanalytical and Nuclear Chemistry, Vol. 285, Issue 3 https://doi.org/10.1007/s10967-010-0627-0	journal	May 2010
Pre-concentration of short-lived radionuclides using manganese dioxide precipitation from surface waters Burnett, J. L.; Croudace, I. W.; Warwick, P. E. Journal of Radioanalytical and Nuclear Chemistry, Vol. 292, Issue 1 https://doi.org/10.1007/s10967-011-1392-4	journal	August 2011
Polymer-coated magnetic nanoparticles for rapid bioassay of 90Sr in human urine samples Varve, Zack; Lai, Edward P. C.; Li, Chunsheng Journal of Radioanalytical and Nuclear Chemistry, Vol. 292, Issue 3 https://doi.org/10.1007/s10967-012-1621-5	journal	January 2012
Application of magnetic nanoparticles for the extraction of radium-226 from water samples Mesnic, Natalie; Sadi, Baki; Li, Chunsheng Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 3 https://doi.org/10.1007/s10967-013-2604-x	journal	July 2013
Selective extraction of 90Sr in urine using 4′4″(5″)di-tert-butyl dicyclohexano-18-crown-6 ether immobilized on polyacrylamide-coated magnetic nanoparticles Varve, Zack; Lai, Edward P. C.; Li, Chunsheng Journal of Radioanalytical and Nuclear Chemistry, Vol. 303, Issue 1 https://doi.org/10.1007/s10967-014-3605-0	journal	September 2014
Magnetic recovery of radium, lead and polonium from seawater samples after preconcentration on a magnetic adsorbent of manganese dioxide coated magnetite Towler, Philip H.; Smith, J. David; Dixon, David R. Analytica Chimica Acta, Vol. 328, Issue 1 https://doi.org/10.1016/0003-2670(96)00080-3	journal	July 1996
Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model Hsi, Ching-kuo Daniel; Langmuir, Donald Geochimica et Cosmochimica Acta, Vol. 49, Issue 9, p. 1931-1941 https://doi.org/10.1016/0016-7037(85)90088-2	journal	September 1985
The behavior of scavenged isotopes in marine anoxic environments: 210Pb and 210Po in the water column of the Black Sea Wei, Ching-Ling; Murray, James W. Geochimica et Cosmochimica Acta, Vol. 58, Issue 7 https://doi.org/10.1016/0016-7037(94)90537-1	journal	April 1994
The surface chemistry of hydrous manganese dioxide Murray, James W. Journal of Colloid and Interface Science, Vol. 46, Issue 3 https://doi.org/10.1016/0021-9797(74)90045-9	journal	March 1974
Solvent extraction study on the hydrolysis of tracer concentration of Po(IV) in chloride solutions Suganuma, Hideo; Hataye, Itsuhachiro Journal of Inorganic and Nuclear Chemistry, Vol. 43, Issue 10 https://doi.org/10.1016/0022-1902(81)80292-8	journal	January 1981
Magnetite surface charge studies to 290°C from in situ pH titrations Wesolowski, David J.; Machesky, Michael L.; Palmer, Donald A. Chemical Geology, Vol. 167, Issue 1-2 https://doi.org/10.1016/S0009-2541(99)00209-0	journal	June 2000
Environmental actinide chemistry Allard, B.; Olofsson, U.; Torstenfelt, B. Inorganica Chimica Acta, Vol. 94, Issue 4 https://doi.org/10.1016/S0020-1693(00)88006-8	journal	April 1984
The point of zero charge of manganese dioxides Gray, M. J.; Malati, M. A.; rophael, M. W. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 89, Issue 1 https://doi.org/10.1016/S0022-0728(78)80038-2	journal	May 1978
Removal of arsenic from groundwater using low cost ferruginous manganese ore Chakravarty, S.; Dureja, V.; Bhattacharyya, G. Water Research, Vol. 36, Issue 3, p. 625-632 https://doi.org/10.1016/S0043-1354(01)00234-2	journal	February 2002
Uranium speciation in waters of different uranium mining areas Bernhard, G.; Geipel, G.; Brendler, V. Journal of Alloys and Compounds, Vol. 271-273 https://doi.org/10.1016/S0925-8388(98)00054-1	journal	June 1998
Modelling americium sorption onto colloids: effect of redox potential Alonso, U.; Degueldre, C. Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 217, Issue 1-3 https://doi.org/10.1016/S0927-7757(02)00558-7	journal	April 2003
Pre-concentration of actinoids from waters: a comparison of various sorbents Koulouris, G.; Slowikowski, B.; Pilviö, R. Applied Radiation and Isotopes, Vol. 53, Issue 1-2 https://doi.org/10.1016/S0969-8043(00)00187-1	journal	July 2000
Preconcentration of radium isotopes from natural waters using MnO2 Resin Moon, D. S.; Burnett, W. C.; Nour, S. Applied Radiation and Isotopes, Vol. 59, Issue 4 https://doi.org/10.1016/S0969-8043(03)00193-3	journal	October 2003
Magnetic solids in analytical chemistry: A review Aguilar-Arteaga, K.; Rodriguez, J. A.; Barrado, E. Analytica Chimica Acta, Vol. 674, Issue 2 https://doi.org/10.1016/j.aca.2010.06.043	journal	August 2010
Preparation and characterization of manganese dioxide impregnated resin for radionuclide pre-concentration Varga, Zsolt Applied Radiation and Isotopes, Vol. 65, Issue 10 https://doi.org/10.1016/j.apradiso.2007.05.001	journal	October 2007
Synthesis of amidoxime-functionalized Fe3O4@SiO2 core–shell magnetic microspheres for highly efficient sorption of U(VI) Zhao, Yingguo; Li, Jiaxing; Zhao, Lanping Chemical Engineering Journal, Vol. 235 https://doi.org/10.1016/j.cej.2013.09.034	journal	January 2014
A surface structural model for ferrihydrite II: Adsorption of uranyl and carbonate Hiemstra, Tjisse; Riemsdijk, Willem H. Van; Rossberg, André Geochimica et Cosmochimica Acta, Vol. 73, Issue 15 https://doi.org/10.1016/j.gca.2009.04.035	journal	August 2009
Adsorption characteristics of 210Pb, 210Po and 7Be onto micro-particle surfaces and the effects of macromolecular organic compounds Yang, Weifeng; Guo, Laodong; Chuang, Chia-Ying Geochimica et Cosmochimica Acta, Vol. 107 https://doi.org/10.1016/j.gca.2012.12.039	journal	April 2013
Cobalt- and manganese-substituted ferrites as efficient single-site heterogeneous catalysts for aerobic oxidation of monoterpenic alkenes under solvent-free conditions Menini, L.; Pereira, M.; Parreira, L. Journal of Catalysis, Vol. 254, Issue 2 https://doi.org/10.1016/j.jcat.2008.01.013	journal	March 2008
Removal of heavy metal ions from aqueous solution using Fe3O4–SiO2-poly(1,2-diaminobenzene) core–shell sub-micron particles Zhang, Fan; Lan, Jing; Zhao, Zongshan Journal of Colloid and Interface Science, Vol. 387, Issue 1 https://doi.org/10.1016/j.jcis.2012.07.066	journal	December 2012
Polonium-210 and lead-210 in the terrestrial environment: a historical review Persson, Bertil R. R.; Holm, Elis Journal of Environmental Radioactivity, Vol. 102, Issue 5 https://doi.org/10.1016/j.jenvrad.2011.01.005	journal	May 2011
Heavy metal removal from water/wastewater by nanosized metal oxides: A review Hua, Ming; Zhang, Shujuan; Pan, Bingcai Journal of Hazardous Materials, Vol. 211-212 https://doi.org/10.1016/j.jhazmat.2011.10.016	journal	April 2012
Functionalized magnetic mesoporous silica nanoparticles for U removal from low and high pH groundwater Li, Dien; Egodawatte, Shani; Kaplan, Daniel I. Journal of Hazardous Materials, Vol. 317 https://doi.org/10.1016/j.jhazmat.2016.05.093	journal	November 2016
Actinide speciation in aquatic systems Choppin, Gregory R. Marine Chemistry, Vol. 99, Issue 1-4 https://doi.org/10.1016/j.marchem.2005.03.011	journal	March 2006
Environmental actinide chemistry Allard, B.; Olofsson, U.; Torstenfelt, B. Inorganica Chimica Acta, Vol. 94, Issue 1-3 https://doi.org/10.1016/s0020-1693(00)94504-3	journal	February 1984
Nanostructured Metal Oxide Sorbents for the Collection and Recovery of Uranium from Seawater Chouyyok, Wilaiwan; Warner, Cynthia L.; Mackie, Katherine E. Industrial & Engineering Chemistry Research, Vol. 55, Issue 15 https://doi.org/10.1021/acs.iecr.5b03650	journal	December 2015
Chemical Insight into the Adsorption of Chromium(III) on Iron Oxide/Mesoporous Silica Nanocomposites Egodawatte, Shani; Datt, Ashish; Burns, Eric A. Langmuir, Vol. 31, Issue 27 https://doi.org/10.1021/acs.langmuir.5b01483	journal	July 2015
Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry Clark, David L.; Hobart, David E.; Neu, Mary P. Chemical Reviews, Vol. 95, Issue 1 https://doi.org/10.1021/cr00033a002	journal	January 1995
Mineral–Water Interface Reactions of Actinides Geckeis, Horst; Lützenkirchen, Johannes; Polly, Robert Chemical Reviews, Vol. 113, Issue 2 https://doi.org/10.1021/cr300370h	journal	October 2012
The Isoelectric Points of Solid Oxides, Solid Hydroxides, and Aqueous Hydroxo Complex Systems Parks, George A. Chemical Reviews, Vol. 65, Issue 2 https://doi.org/10.1021/cr60234a002	journal	April 1965
Influence of Calcite and Dissolved Calcium on Uranium(VI) Sorption to a Hanford Subsurface Sediment Dong, Wenming; Ball, William P.; Liu, Chongxuan Environmental Science & Technology, Vol. 39, Issue 20 https://doi.org/10.1021/es0505088	journal	October 2005
Sorption of Am(III) onto 6-Line-Ferrihydrite and Its Alteration Products: Investigations by EXAFS Stumpf, Silvia; Stumpf, Thorsten; Dardenne, Kathy Environmental Science & Technology, Vol. 40, Issue 11 https://doi.org/10.1021/es052518e	journal	June 2006
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 Dong, Wenming; Brooks, Scott C. Environmental Science & Technology, Vol. 40, Issue 15 https://doi.org/10.1021/es0606327	journal	August 2006
Conjugates of Magnetic Nanoparticle—Actinide Specific Chelator for Radioactive Waste Separation Kaur, Maninder; Zhang, Huijin; Martin, Leigh Environmental Science & Technology, Vol. 47, Issue 21 https://doi.org/10.1021/es402205q	journal	October 2013
Cation sorption on colloidal hydrous manganese dioxide Posselt, Hans S.; Anderson, Frederick J.; Weber, Walter J. Environmental Science & Technology, Vol. 2, Issue 12 https://doi.org/10.1021/es60023a005	journal	December 1968
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 Tamura, Hiroki; Katayama, Noriaki; Furuichi, Ryusaburo Environmental Science & Technology, Vol. 30, Issue 4 https://doi.org/10.1021/es9504404	journal	January 1996
Effect of Crystallographic Structure of MnO ₂ on Its Electrochemical Capacitance Properties Devaraj, S.; Munichandraiah, N. The Journal of Physical Chemistry C, Vol. 112, Issue 11 https://doi.org/10.1021/jp7108785	journal	February 2008
Synthesis of Highly Selective Magnetic Mesoporous Adsorbent Chen, Xinqing; Lam, Koon Fung; Zhang, Qingjian The Journal of Physical Chemistry C, Vol. 113, Issue 22 https://doi.org/10.1021/jp9018052	journal	May 2009
Manganese Doping of Magnetic Iron Oxide Nanoparticles: Tailoring Surface Reactivity for a Regenerable Heavy Metal Sorbent Warner, Cynthia L.; Chouyyok, Wilaiwan; Mackie, Katherine E. Langmuir, Vol. 28, Issue 8 https://doi.org/10.1021/la2042235	journal	February 2012
Extraction of radium from natural waters using manganese-impregnated acrylic fibers Moore, Willard S.; Reid, David F. Journal of Geophysical Research, Vol. 78, Issue 36 https://doi.org/10.1029/JC078i036p08880	journal	December 1973
Bare magnetic nanoparticles: sustainable synthesis and applications in catalytic organic transformations Hudson, Reuben; Feng, Yuting; Varma, Rajender S. Green Chem., Vol. 16, Issue 10 https://doi.org/10.1039/C4GC00418C	journal	January 2014
Chelate-free metal ion binding and heat-induced radiolabeling of iron oxide nanoparticles Boros, Eszter; Bowen, Alice M.; Josephson, Lee Chemical Science, Vol. 6, Issue 1 https://doi.org/10.1039/C4SC02778G	journal	January 2015
First-principles molecular dynamics simulation of the Ca ₂ UO ₂ (CO ₃ ) ₃ complex in water Priest, Chad; Tian, Ziqi; Jiang, De-en Dalton Transactions, Vol. 45, Issue 24 https://doi.org/10.1039/C5DT04576B	journal	January 2016
Magnetic nanoparticle-supported crown ethers Kawamura, Masato; Sato, Kazuhiko Chemical Communications, Issue 32 https://doi.org/10.1039/b705640k	journal	January 2007
Functionalized Magnetite Nanoparticles—Synthesis, Properties, and Bio-Applications Majewski, Peter; Thierry, Benjamin Critical Reviews in Solid State and Materials Sciences, Vol. 32, Issue 3-4 https://doi.org/10.1080/10408430701776680	journal	December 2007
Synthesis and ion Exchange Properties of Manganese(Iv) Dioxide Doped by 3+ Transition Metal Cations Bartoś, Barbara; Bilewicz, Aleksander Solvent Extraction and Ion Exchange, Vol. 19, Issue 3 https://doi.org/10.1081/SEI-100103285	journal	May 2001
EURADOS intercomparison on emergency radiobioassay Li, Chunsheng; Battisti, Paolo; Berard, Philippe Radiation Protection Dosimetry, Vol. 167, Issue 4 https://doi.org/10.1093/rpd/ncu366	journal	December 2014
International Workshop on Emergency Radiobioassay: Considerations, gaps and Recommendations Li, Chunsheng; Inn, Kenneth G. W.; Jones, Robert Health Physics, Vol. 101, Issue 2 https://doi.org/10.1097/HP.0b013e318213a5da	journal	January 2011
Investigation of Magnetic Nanoparticles for the Rapid Extraction and Assay of Alpha-Emitting Radionuclides from Urine: Demonstration of a Novel Radiobioassay Method OʼHara, Matthew J.; Carter, Jennifer C.; MacLellan, Jay A. Health Physics, Vol. 101, Issue 2 https://doi.org/10.1097/HP.0b013e3182166ed1	journal	January 2011
Preparation of catalysts by metallic complex adsorption on mineral oxides Brunelle, J. P. Pure and Applied Chemistry, Vol. 50, Issue 9-10 https://doi.org/10.1351/pac197850091211	journal	January 1978
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 Ulrich, H. J.; Degueldre, C. Radiochimica Acta, Vol. 62, Issue 1-2 https://doi.org/10.1524/ract.1993.62.12.81	journal	January 1993
Sorption of 241Am onto Montmorillonite, Illite and Hematite Colloids Degueldre, C.; Ulrich, H. J. .; Silby, H. Radiochimica Acta, Vol. 65, Issue 3 https://doi.org/10.1524/ract.1994.65.3.173	journal	January 1994
Soluble and Particle-Bound and 210Po 210Pb in Groundwaters Lehto, J.; Kelokaski, P.; Vaaramaa, K. Radiochimica Acta, Vol. 85, Issue 3-4 https://doi.org/10.1524/ract.1999.85.34.149	journal	January 1999
Identification and characterization of sorbed lutetium species on 2-line ferrihydrite by sorption data modeling, TRLFS and EXAFS Dardenne, K.; Schäfer, T.; Denecke, Melissa A. Radiochimica Acta, Vol. 89, Issue 7 https://doi.org/10.1524/ract.2001.89.7.469	journal	January 2001
Soluble and particle-bound 234,238U, 226Ra and 210Po in ground waters Vaaramaa, K.; Lehto, J.; Ervanne, H. Radiochimica Acta, Vol. 91, Issue 1 https://doi.org/10.1524/ract.91.1.21.19015	journal	January 2003
Plutonium and Americium Geochemistry at Hanford: A Site Wide Review Cantrell, Kirk J.; Felmy, Andrew R. https://doi.org/10.2172/1051201	report	August 2012
Imaging in Clinical Oncology Kim, E. E. Journal of Nuclear Medicine, Vol. 56, Issue 4 https://doi.org/10.2967/jnumed.115.155523	journal	February 2015
Imaging in Clinical Oncology Kim, E. E. Journal of Nuclear Medicine https://doi.org/10.2967/jnumed.115.157453	journal	April 2015

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