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

Title: 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:1339852

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

Magnetic nanoparticles are well known to possess chemically active surfaces and high surface areas that can be employed to extract a range of ions from aqueous solutions. Additionally, their paramagnetic property provides 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 both naturally occurring radioactive isotopes (polonium (Po), radium (Ra), and uranium (U)) as well as the transuranic element americium (Am) from a suite of naturally occurring aqueous matrices. The nanomaterials include commercially available paramagnetic magnetite (Fe3O4) and magnetite that was 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 (acidified with HCl). 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 aforementioned alpha-emitting radionuclide spikes from Hanford Site 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. 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 groundwater 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. These applications may include analytical chemistry, waste water treatment and remediation, mining, and in vitro radiobioassay.

Cite

Export

Save

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

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1339852

Report Number(s):: PNNL-SA-119737; RSCACL; 400412000

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

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

References (67)

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
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
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
Magnetic nanoparticle-supported crown ethers Kawamura, Masato; Sato, Kazuhiko Chemical Communications, Issue 32 https://doi.org/10.1039/b705640k	journal	January 2007
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
�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 Kim, E. E. Journal of Nuclear Medicine, Vol. 56, Issue 4 https://doi.org/10.2967/jnumed.115.155523	journal	February 2015
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
Imaging in Clinical Oncology Kim, E. E. Journal of Nuclear Medicine https://doi.org/10.2967/jnumed.115.157453	journal	April 2015
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

Cited By (1)

Transforming lanthanide and actinide chemistry with nanoparticles Pallares, Roger M.; Abergel, Rebecca J. Nanoscale, Vol. 12, Issue 3 https://doi.org/10.1039/c9nr09175k	journal	January 2020

Similar Records

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 · OSTI ID:1339852

O'Hara, Matthew J.; Carter, Jennifer C.; Warner, Cynthia L.; +2 more

Testing the stability of magnetic iron oxides/kaolinite nanocomposite under various pH conditions

Journal Article · Fri Sep 15 00:00:00 EDT 2017 · Journal of Solid State Chemistry · OSTI ID:1339852

Tokarčíková, Michaela; Tokarský, Jonáš; Kutláková, Kateřina Mamulová; +1 more

Effective Media for Immobilising and Isolating Radionuclides from Aqueous Nuclear Wastes: Reaction Products of Bone Char and Uranyl Ions

Conference · Sat Jul 01 00:00:00 EDT 2006 · OSTI ID:1339852

Warwick, P E; Croudace, I W; Holland, N G; +2 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Magnetite
MnO2
NORM
bioassay
remediation
waste treatment
radiochemistry
mineral-water interface
magnetic separations

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

Citation Formats

References (67)

Cited By (1)

Similar Records

Related Subjects