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Title: Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings

Abstract

Herein, we describe engineered superparamagnetic iron oxide nanoparticles (IONPs) as platform materials for enhanced uranyl (UO22+) sorption and separation processes under environmentally relevant conditions. Specifically, monodispersed 8-25 nm iron oxide (magnetite, Fe3O4) nanoparticles with tailored organic acid bilayered coatings have been systematically evaluated and optimized to bind, and thus remove, uranium from water. The combined nonhydrolytic synthesis and bilayer phase transfer material preparation methods yield highly uniform and surface tailorable IONPs, which allow for direct evaluation of the size-dependent and coating-dependent sorption capacities of IONPs. Optimized materials demonstrate ultrahigh sorption capacities (>50% by wt/wt) at pH 5.6 for 8 nm oleic acid (OA) bilayer and sodium monododecyl phosphate (SDP) surface-stabilized IONPs. Synchrotron-based X-ray absorption spectroscopy shows that iron oxide core particle size and stabilizing surface functional group(s) substantially affect U(VI)-removal mechanisms, specifically the ratio of uptake via adsorption versus reduction to U(IV). Taken together, tunable size and surface functionality, high colloidal stability, and favorable affinity toward uranium provide distinct synergistic advantage(s) for the application of bilayered IONPs as part of the next-generation material-based uranium recovery, remediation, and sensing technologies

Authors:
ORCiD logo; ; ; ; ;  [1]; ;
  1. U.S. Army Corps of Engineers, Engineer Research and Development Center, Vicksburg, Mississippi 39180, United States
Publication Date:
Research Org.:
Washington Univ., St. Louis, MO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1415163
Alternate Identifier(s):
OSTI ID: 1356408; OSTI ID: 1508035
Grant/Contract Number:  
SC0006857
Resource Type:
Published Article
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Name: ACS Applied Materials and Interfaces Journal Volume: 9 Journal Issue: 15; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; bilayer surface coating; critical coagulation concentration; environmental remediation; iron oxide nanoparticles (IONPs); nanoparticle stability; uranium reduction; uranium sorption; XAFS; iron oxide nanoparticles (IONPs), nanoparticle stability, bilayer surface coating, critical coagulation concentration, uranium sorption, uranium reduction, environmental remediation, XAFS

Citation Formats

Li, Wenlu, Troyer, Lyndsay D., Lee, Seung Soo, Wu, Jiewei, Kim, Changwoo, Lafferty, Brandon J., Catalano, Jeffrey G., and Fortner, John D. Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings. United States: N. p., 2017. Web. doi:10.1021/acsami.7b01042.
Li, Wenlu, Troyer, Lyndsay D., Lee, Seung Soo, Wu, Jiewei, Kim, Changwoo, Lafferty, Brandon J., Catalano, Jeffrey G., & Fortner, John D. Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings. United States. https://doi.org/10.1021/acsami.7b01042
Li, Wenlu, Troyer, Lyndsay D., Lee, Seung Soo, Wu, Jiewei, Kim, Changwoo, Lafferty, Brandon J., Catalano, Jeffrey G., and Fortner, John D. Tue . "Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings". United States. https://doi.org/10.1021/acsami.7b01042.
@article{osti_1415163,
title = {Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings},
author = {Li, Wenlu and Troyer, Lyndsay D. and Lee, Seung Soo and Wu, Jiewei and Kim, Changwoo and Lafferty, Brandon J. and Catalano, Jeffrey G. and Fortner, John D.},
abstractNote = {Herein, we describe engineered superparamagnetic iron oxide nanoparticles (IONPs) as platform materials for enhanced uranyl (UO22+) sorption and separation processes under environmentally relevant conditions. Specifically, monodispersed 8-25 nm iron oxide (magnetite, Fe3O4) nanoparticles with tailored organic acid bilayered coatings have been systematically evaluated and optimized to bind, and thus remove, uranium from water. The combined nonhydrolytic synthesis and bilayer phase transfer material preparation methods yield highly uniform and surface tailorable IONPs, which allow for direct evaluation of the size-dependent and coating-dependent sorption capacities of IONPs. Optimized materials demonstrate ultrahigh sorption capacities (>50% by wt/wt) at pH 5.6 for 8 nm oleic acid (OA) bilayer and sodium monododecyl phosphate (SDP) surface-stabilized IONPs. Synchrotron-based X-ray absorption spectroscopy shows that iron oxide core particle size and stabilizing surface functional group(s) substantially affect U(VI)-removal mechanisms, specifically the ratio of uptake via adsorption versus reduction to U(IV). Taken together, tunable size and surface functionality, high colloidal stability, and favorable affinity toward uranium provide distinct synergistic advantage(s) for the application of bilayered IONPs as part of the next-generation material-based uranium recovery, remediation, and sensing technologies},
doi = {10.1021/acsami.7b01042},
journal = {ACS Applied Materials and Interfaces},
number = 15,
volume = 9,
place = {United States},
year = {Tue Apr 04 00:00:00 EDT 2017},
month = {Tue Apr 04 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1021/acsami.7b01042

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Works referenced in this record:

Extracellular reduction of uranium via Geobacter conductive pili as a protective cellular mechanism
journal, September 2011

  • Cologgi, D. L.; Lampa-Pastirk, S.; Speers, A. M.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 37, p. 15248-15252
  • DOI: 10.1073/pnas.1108616108

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Removal of uranium(VI) from the aqueous phase by iron(II) minerals in presence of bicarbonate
journal, September 2009


Influence of Dynamical Conditions on the Reduction of U VI at the Magnetite−Solution Interface
journal, January 2010

  • Ilton, Eugene S.; Boily, Jean-François; Buck, Edgar C.
  • Environmental Science & Technology, Vol. 44, Issue 1
  • DOI: 10.1021/es9014597

Simultaneous reduction and adsorption for immobilization of uranium from aqueous solution by nano-flake Fe-SC
journal, December 2016


Synthesis of Monodisperse Spherical Nanocrystals
journal, June 2007

  • Park, Jongnam; Joo, Jin; Kwon, Soon Gu
  • Angewandte Chemie International Edition, Vol. 46, Issue 25
  • DOI: 10.1002/anie.200603148

Colorimetric Peroxidase Mimetic Assay for Uranyl Detection in Sea Water
journal, February 2015

  • Zhang, Dingyuan; Chen, Zhuo; Omar, Haneen
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 8
  • DOI: 10.1021/am507361x

Aqueous Aggregation and Surface Deposition Processes of Engineered Superparamagnetic Iron Oxide Nanoparticles for Environmental Applications
journal, October 2014

  • Li, Wenlu; Liu, Di; Wu, Jiewei
  • Environmental Science & Technology, Vol. 48, Issue 20
  • DOI: 10.1021/es502174p

U(VI) Reduction to Mononuclear U(IV) by Desulfitobacterium Species
journal, June 2010

  • Fletcher, Kelly E.; Boyanov, Maxim I.; Thomas, Sara H.
  • Environmental Science & Technology, Vol. 44, Issue 12
  • DOI: 10.1021/es903636c

Removal of uranium(VI) from aqueous solutions by nanoporous carbon and its chelating polymer composite
journal, May 2010

  • Kim, Jin Hoe; Lee, Hyung Ik; Yeon, Jei-Won
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 286, Issue 1
  • DOI: 10.1007/s10967-010-0624-3

Magnetic Iron Oxide Nanoparticles: Synthesis, Stabilization, Vectorization, Physicochemical Characterizations, and Biological Applications
journal, June 2008

  • Laurent, Sophie; Forge, Delphine; Port, Marc
  • Chemical Reviews, Vol. 108, Issue 6, p. 2064-2110
  • DOI: 10.1021/cr068445e

Reduction of U(VI) to U(IV) on the surface of magnetite
journal, December 2005


Low-Field Magnetic Separation of Monodisperse Fe3O4 Nanocrystals
journal, November 2006


Uranium(VI) Solubility and Speciation in Simulated Elemental Human Biological Fluids
journal, November 2004

  • Sutton, Mark; Burastero, Stephen R.
  • Chemical Research in Toxicology, Vol. 17, Issue 11
  • DOI: 10.1021/tx049878k

Preparation and application of attapulgite/iron oxide magnetic composites for the removal of U(VI) from aqueous solution
journal, September 2011


Removal of Heavy Metals from Aqueous Systems with Thiol Functionalized Superparamagnetic Nanoparticles
journal, July 2007

  • Yantasee, Wassana; Warner, Cynthia L.; Sangvanich, Thanapon
  • Environmental Science & Technology, Vol. 41, Issue 14
  • DOI: 10.1021/es0705238

Shape and size controlled synthesis of uniform iron oxide nanocrystals through new non-hydrolytic routes
journal, June 2016


Reductive immobilization of uranium by PAAM–FeS/Fe 3 O 4 magnetic composites
journal, January 2015

  • Shao, Dadong; Wang, Xiangxue; Li, Jiaxing
  • Environmental Science: Water Research & Technology, Vol. 1, Issue 2
  • DOI: 10.1039/C4EW00014E

Engineered superparamagnetic iron oxide nanoparticles for ultra-enhanced uranium separation and sensing
journal, January 2016

  • Li, Wenlu; Mayo, John T.; Benoit, Denise N.
  • Journal of Materials Chemistry A, Vol. 4, Issue 39
  • DOI: 10.1039/C6TA04709B

Development of a Functionalized Polymer-Coated Silica for the Removal of Uranium from Groundwater
journal, September 2003

  • Bryant, David E.; Stewart, Douglas I.; Kee, Terence P.
  • Environmental Science & Technology, Vol. 37, Issue 17
  • DOI: 10.1021/es020178g

Evidence for multiple modes of uranium immobilization by an anaerobic bacterium
journal, May 2011

  • Ray, Allison E.; Bargar, John R.; Sivaswamy, Vaideeswaran
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 10
  • DOI: 10.1016/j.gca.2011.02.040

Non-uraninite Products of Microbial U(VI) Reduction
journal, December 2010

  • Bernier-Latmani, Rizlan; Veeramani, Harish; Vecchia, Elena Dalla
  • Environmental Science & Technology, Vol. 44, Issue 24
  • DOI: 10.1021/es101675a

Association of Uranium with Iron Oxides Typically Formed on Corroding Steel Surfaces
journal, July 2002

  • Dodge, C. J.; Francis, A. J.; Gillow, J. B.
  • Environmental Science & Technology, Vol. 36, Issue 16
  • DOI: 10.1021/es011450+

Sorption of uranium(VI) from aqueous solutions by akaganeite
journal, December 2008


Uranium (VI) recovery from aqueous medium using novel floating macroporous alginate-agarose-magnetite cryobeads
journal, February 2013


Quantitative Separation of Monomeric U(IV) from UO 2 in Products of U(VI) Reduction
journal, May 2012

  • Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish
  • Environmental Science & Technology, Vol. 46, Issue 11
  • DOI: 10.1021/es204123z

Uranyl adsorption onto montmorillonite: Evaluation of binding sites and carbonate complexation
journal, June 2005


Impact of water quality parameters on the sorption of U(VI) onto hematite
journal, January 2012


Carbonate Effects on Hexavalent Uranium Adsorption by Iron Oxyhydroxide
journal, August 2003

  • Wazne, Mahmoud; Korfiatis, George P.; Meng, Xiaoguang
  • Environmental Science & Technology, Vol. 37, Issue 16
  • DOI: 10.1021/es034166m

Efficient Uranium Capture by Polysulfide/Layered Double Hydroxide Composites
journal, March 2015

  • Ma, Shulan; Huang, Lu; Ma, Lijiao
  • Journal of the American Chemical Society, Vol. 137, Issue 10
  • DOI: 10.1021/jacs.5b00762

Enrichment and Encapsulation of Uranium with Iron Nanoparticle
journal, February 2015

  • Ling, Lan; Zhang, Wei-xian
  • Journal of the American Chemical Society, Vol. 137, Issue 8
  • DOI: 10.1021/ja510488r

Synthesis of Fe3O4@TiO2 core–shell magnetic composites for highly efficient sorption of uranium (VI)
journal, March 2015


Synthesis of amidoxime-functionalized Fe3O4@SiO2 core–shell magnetic microspheres for highly efficient sorption of U(VI)
journal, January 2014


Nanoscale Size Effects on Uranium(VI) Adsorption to Hematite
journal, March 2009

  • Zeng, Hui; Singh, Abhas; Basak, Soubir
  • Environmental Science & Technology, Vol. 43, Issue 5
  • DOI: 10.1021/es802334e

Rapid removal of uranium from aqueous solutions using magnetic Fe3O4@SiO2 composite particles
journal, April 2012


Adsorption of Uranium(VI) to Manganese Oxides: X-ray Absorption Spectroscopy and Surface Complexation Modeling
journal, December 2012

  • Wang, Zimeng; Lee, Sung-Woo; Catalano, Jeffrey G.
  • Environmental Science & Technology, Vol. 47, Issue 2
  • DOI: 10.1021/es304454g

Magnesium oxide nanoparticles: Preparation, characterization, and uranium sorption properties
journal, July 2011

  • Camtakan, Zeyneb; Erenturk, Sema Akyil; Yusan, Sabriye Doyurum
  • Environmental Progress & Sustainable Energy, Vol. 31, Issue 4
  • DOI: 10.1002/ep.10575

Bilayers as Phase Transfer Agents for Nanocrystals Prepared in Nonpolar Solvents
journal, July 2009

  • Prakash, Arjun; Zhu, Huiguang; Jones, Christopher J.
  • ACS Nano, Vol. 3, Issue 8
  • DOI: 10.1021/nn900373b

Engineered manganese oxide nanocrystals for enhanced uranyl sorption and separation
journal, January 2015

  • Lee, Seung Soo; Li, Wenlu; Kim, Changwoo
  • Environmental Science: Nano, Vol. 2, Issue 5
  • DOI: 10.1039/C5EN00010F

Synthesis and application of magnetic graphene/iron oxides composite for the removal of U(VI) from aqueous solutions
journal, March 2013


Products of abiotic U(VI) reduction by biogenic magnetite and vivianite
journal, May 2011

  • Veeramani, Harish; Alessi, Daniel S.; Suvorova, Elena I.
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 9
  • DOI: 10.1016/j.gca.2011.02.024

Magnetite and zero-valent iron nanoparticles for the remediation of uranium contaminated environmental water
journal, April 2011


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
  • DOI: 10.1007/s10967-010-0627-0

Multiple mechanisms of uranium immobilization by Cellulomonas sp. strain ES6
journal, October 2010

  • Sivaswamy, Vaideeswaran; Boyanov, Maxim I.; Peyton, Brent M.
  • Biotechnology and Bioengineering, Vol. 108, Issue 2
  • DOI: 10.1002/bit.22956

Efficient Removal and Recovery of Uranium by a Layered Organic–Inorganic Hybrid Thiostannate
journal, September 2016

  • Feng, Mei-Ling; Sarma, Debajit; Qi, Xing-Hui
  • Journal of the American Chemical Society, Vol. 138, Issue 38
  • DOI: 10.1021/jacs.6b07351

Use of iron oxide nanomaterials in wastewater treatment: A review
journal, May 2012


Pore-Free Matrix with Cooperative Chelating of Hyperbranched Ligands for High-Performance Separation of Uranium
journal, October 2016

  • Li, Yang; Wang, Lei; Li, Bo
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 42
  • DOI: 10.1021/acsami.6b09681

Aqueous Aggregation Behavior of Engineered Superparamagnetic Iron Oxide Nanoparticles: Effects of Oxidative Surface Aging
journal, November 2016

  • Li, Wenlu; Lee, Seung Soo; Mittelman, Anjuliee M.
  • Environmental Science & Technology, Vol. 50, Issue 23
  • DOI: 10.1021/acs.est.6b04130

High Temperature Decomposition of Cerium Precursors To Form Ceria Nanocrystal Libraries for Biological Applications
journal, December 2011

  • Lee, Seung Soo; Zhu, Huiguang; Contreras, Elizabeth Q.
  • Chemistry of Materials, Vol. 24, Issue 3
  • DOI: 10.1021/cm200863q

Solution and Microbial Controls on the Formation of Reduced U(IV) Species
journal, October 2011

  • Boyanov, Maxim I.; Fletcher, Kelly E.; Kwon, Man Jae
  • Environmental Science & Technology, Vol. 45, Issue 19
  • DOI: 10.1021/es2014049

The design and utility of polymer-stabilized iron-oxide nanoparticles for nanomedicine applications
journal, January 2010

  • Boyer, Cyrille; Whittaker, Michael R.; Bulmus, Volga
  • NPG Asia Materials, Vol. 2, Issue 1
  • DOI: 10.1038/asiamat.2010.6

Amidoxime-modified mesoporous silica for uranium adsorption under seawater conditions
journal, January 2015

  • Gunathilake, Chamila; Górka, Joanna; Dai, Shen
  • Journal of Materials Chemistry A, Vol. 3, Issue 21
  • DOI: 10.1039/C5TA02863A

A DNAzyme-Gold Nanoparticle Probe for Uranyl Ion in Living Cells
journal, March 2013

  • Wu, Peiwen; Hwang, Kevin; Lan, Tian
  • Journal of the American Chemical Society, Vol. 135, Issue 14
  • DOI: 10.1021/ja400150v

Characterization of U(VI)-carbonato ternary complexes on hematite: EXAFS and electrophoretic mobility measurements
journal, August 2000


Amino Acid Functionalized Chitosan Magnetic Nanobased Particles for Uranyl Sorption
journal, December 2015

  • Galhoum, Ahmed A.; Mahfouz, Mohammad G.; Atia, Asem A.
  • Industrial & Engineering Chemistry Research, Vol. 54, Issue 49
  • DOI: 10.1021/acs.iecr.5b03331

Recycling of Uranyl from Contaminated Water
journal, September 2013

  • Bohinc, Klemen; Reščič, Jurij; Dufreche, Jean-Francois
  • The Journal of Physical Chemistry B, Vol. 117, Issue 37
  • DOI: 10.1021/jp404822f

Simultaneous adsorption and reduction of U(VI) on reduced graphene oxide-supported nanoscale zerovalent iron
journal, September 2014


A Biocompatible Method of Decorporation:  Bisphosphonate-Modified Magnetite Nanoparticles to Remove Uranyl Ions from Blood
journal, October 2006

  • Wang, Ling; Yang, Zhimou; Gao, Jinhao
  • Journal of the American Chemical Society, Vol. 128, Issue 41
  • DOI: 10.1021/ja0651355

Surface engineering superparamagnetic nanoparticles for aqueous applications: design and characterization of tailored organic bilayers
journal, January 2016

  • Li, Wenlu; Hinton, Carl H.; Lee, Seung Soo
  • Environmental Science: Nano, Vol. 3, Issue 1
  • DOI: 10.1039/C5EN00089K

IFEFFIT  : interactive XAFS analysis and FEFF fitting
journal, March 2001


Experimental determination of UO2(cr) dissolution kinetics: Effects of solution saturation state and pH
journal, October 2005


Uranium redox transition pathways in acetate-amended sediments
journal, March 2013

  • Bargar, J. R.; Williams, K. H.; Campbell, K. M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 12
  • DOI: 10.1073/pnas.1219198110