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

Here, we describe engineered superparamagnetic iron oxide nanoparticles (IONPs) as platform materials for enhanced uranyl (UO 2 2+) sorption and separation processes under environmentally relevant conditions. Specifically, monodispersed 8–25 nm iron oxide (magnetite, Fe 3O 4) 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] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1]
  1. Washington Univ. in St. Louis, St. Louis, MO (United States)
  2. U.S. Army Corps of Engineers, Vicksburg, MS (United States)
Publication Date:
Grant/Contract Number:
SC0006857
Type:
Published Article
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 15; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Research Org:
Washington Univ., St. Louis, MO (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
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
OSTI Identifier:
1415163
Alternate Identifier(s):
OSTI ID: 1356408

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., 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. doi: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.. 2017. "Engineering Nanoscale Iron Oxides for Uranyl Sorption and Separation: Optimization of Particle Core Size and Bilayer Surface Coatings". United States. doi: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 = {Here, 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 = {2017},
month = {3}
}