Sequestration of U(VI) from Acidic, Alkaline, and High Ionic-Strength Aqueous Media by Functionalized Magnetic Mesoporous Silica Nanoparticles: Capacity and Binding Mechanisms

Li, Dien; Egodawatte, Shani; Kaplan, Daniel I.; Larsen, Sarah C.; Serkiz, Steven M.; Seaman, John C.; Scheckel, Kirk G.; Lin, Jinru; Pan, Yuanming

doi:10.1021/acs.est.7b03778

Sequestration of U(VI) from Acidic, Alkaline, and High Ionic-Strength Aqueous Media by Functionalized Magnetic Mesoporous Silica Nanoparticles: Capacity and Binding Mechanisms

Journal Article · Mon Nov 20 00:00:00 EST 2017 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b03778· OSTI ID:1501348

^[1]; Egodawatte, Shani ^[2]; Kaplan, Daniel I. ^[1]; ^[2]; Serkiz, Steven M. ^[1]; Seaman, John C. ^[3]; Scheckel, Kirk G. ^[4]; Lin, Jinru ^[5]; Pan, Yuanming ^[5]

Savannah River National Lab. (SRNL), Aiken, SC (United States).
Univ. of Iowa, Iowa City, IA (United States)
Univ. of Georgia, Aiken, SC (United States). Savannah River Ecology Lab.
US Environmental Protection Agency (EPA), Cincinnati, OH (United States). National Risk Management Research Lab.
Univ. of Saskatchewan, Saskatoon, SK (Canada)

Uranium(VI) exhibits little adsorption onto sediment minerals in acidic, alkaline or high ionic-strength aqueous media that often occur in U mining or contaminated sites, which makes U(VI) very mobile and difficult to sequester. In this work, magnetic mesoporous silica nanoparticles (MMSNs) were functionalized with several organic ligands. The functionalized MMSNs were highly effective and had large binding capacity for U sequestration from high salt water (HSW) simulant (54 mg U/g sorbent). The functionalized MMSNs, after U exposure in HSW simulant, pH 3.5 and 9.6 artificial groundwater (AGW), were characterized by a host of spectroscopic methods. Among the key novel findings in this work was that in the HSW simulant or high pH AGW, the dominant U species bound to the functionalized MMSNs were uranyl or uranyl hydroxide, rather than uranyl carbonates as expected. The surface functional groups appear to be out-competing the carbonate ligands associated with the aqueous U species. The uranyl-like species were bound with N ligand as η² bound motifs or phosphonate ligand as a monodentate, as well as on tetrahedral Si sites as an edge-sharing bidentate. Conclusively, the N and phosphonate ligand-functionalized MMSNs hold promise as effective sorbents for sequestering U from acidic, alkaline or high ionic-strength contaminated aqueous media.

View Accepted Manuscript (DOE)

Research Organization:: Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

Sponsoring Organization:: DOE

Grant/Contract Number:: AC09-08SR22470

OSTI ID:: 1501348

Report Number(s):: SRNL-STI--2017-00262

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 24 Vol. 51; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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