Uranyl Peroxide Nanocluster (U60) Persistence and Sorption in the Presence of Hematite

Sadergaski, Luke R.; Stoxen, Wynn; Hixon, Amy E.

doi:10.1021/acs.est.7b06510

Uranyl Peroxide Nanocluster (U₆₀) Persistence and Sorption in the Presence of Hematite

Journal Article · Tue Feb 13 00:00:00 EST 2018 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b06510· OSTI ID:1470352

Sadergaski, Luke R. ^[1]; Stoxen, Wynn ^[1]; ^[1]

Univ. of Notre Dame, IN (United States). Dept. of Civil and Environmental Engineering and Earth Sciences

The presence of uranium-based nanomaterials in environmental systems may significantly impact our current understanding of the fate and transport of U(VI). Sorption of the uranyl peroxide nanocluster [(UO₂)(O₂)(OH)]₆₀^60– (U₆₀) to hematite (α-Fe₂O₃) was studied using batch sorption experiments with varying U₆₀, hematite, and alkali electrolyte (i.e., NaCl, KCl, and CsCl) concentrations. Data from electrospray ionization mass spectrometry and centrifugal microfiltration revealed that U₆₀ persisted in the presence of hematite and the background electrolyte for at least 120 days. K⁺ ions were removed from solution with uranium whereas Li⁺ ions remained in solution, indicating that the U₆₀ cluster behaved like an anion and that the Li⁺ ions did not play a significant role in the sorption mechanism. Analysis of the reacted mineral surface using X-ray photoelectron and Raman spectroscopies confirmed the presence of U(VI) and uranyl species with bridged peroxo groups associated with the mineral surface. These results indicate that uranyl peroxide nanoclusters may persist in the aqueous phase under environmentally relevant conditions for reasonably long periods of time, as compared to that of the uranyl cation.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Materials Science of Actinides (MSA)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001089

OSTI ID:: 1470352

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 5 Vol. 52; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited By (2)

In situ Raman spectroscopy of uranyl peroxide nanoscale cage clusters under hydrothermal conditions Lobeck, Haylie L.; Traustason, Hrafn; Julien, Patrick A. Dalton Transactions, Vol. 48, Issue 22 https://doi.org/10.1039/c9dt01529a	journal	January 2019
Evidence for non-electrostatic interactions between a pyrophosphate-functionalized uranyl peroxide nanocluster and iron (hydr)oxide minerals Sadergaski, Luke R.; Perry, Samuel N.; Tholen, Luke R. Environmental Science: Processes & Impacts, Vol. 21, Issue 7 https://doi.org/10.1039/c9em00139e	journal	January 2019

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
54 ENVIRONMENTAL SCIENCES
aqueous speciation
hematite
materials and chemistry by design
nuclear (including radiation effects)
sorption
synthesis (novel materials)
synthesis (self-assembly)
uranyl peroxide nanoclusters