Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 9, Issue 15, Pages 13163-13172Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b01042
Keywords
iron oxide nanoparticles (IONPs); nanoparticle stability; bilayer surface coating; critical coagulation concentration; uranium sorption; uranium reduction; environmental remediation; XAFS
Funding
- American Chemical Society's Petroleum Research Fund [52640-DNI10]
- U.S. National Science Foundation (NSF) (CBET) [1236653, 1437820]
- U.S. Army Corps of Engineers [W912HZ-13-2-0009-P00001]
- Department of Energy (DOE) Subsurface Biogeochemical Research Program [DE-SC0006857]
- U.S. NSF [ECS-0335765]
- DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
- U.S. Department of Energy (DOE) [DE-SC0006857] Funding Source: U.S. Department of Energy (DOE)
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1437820] Funding Source: National Science Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1236653] Funding Source: National Science Foundation
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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.
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