Calcium-Facilitated Aggregation and Precipitation of the Uranyl Peroxide Nanocluster U60 in the Presence of Na-Montmorillonite

Sadergaski, Luke R.; Said, Meena; Hixon, Amy E.

doi:10.1021/acs.est.8b06731

Calcium-Facilitated Aggregation and Precipitation of the Uranyl Peroxide Nanocluster U₆₀ in the Presence of Na-Montmorillonite

Journal Article · Thu Mar 28 00:00:00 EDT 2019 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.8b06731· OSTI ID:1566497

Sadergaski, Luke R. ^[1]; Said, Meena ^[1]; ^[1]

Univ. of Notre Dame, Notre Dame, IN (United States)

The unique and diverse features of uranyl peroxide nanoclusters may contribute to the enhanced mobility of uranium in the environment. This study examines the sorption of the uranyl peroxide nanocluster [UO₂(O₂)(OH)]₆₀^60- (U₆₀) to Na-montmorillonite (SWy-2), plagioclase (anorthite), and quartz (SiO₂) as a function of time, U₆₀ concentration, and mineral concentration. SWy-2 was studied in both its untreated form as well as after two different pretreatments, denoted as partially treated SWy-2 and fully treated SWy-2. U₆₀ was removed (~99%) from solution in the presence of untreated and partially treated SWy-2. However, U₆₀ was not removed from suspensions containing anorthite, quartz, or fully treated SWy-2, even after several months. The removal of U₆₀ from suspensions containing untreated SWy-2 is promoted in part by the exchange of Li⁺ counter-ions, normally weakly associated with U₆₀ in solution, for Ca²⁺ ions naturally present in the clay. In solution, Ca²⁺ ions induce the aggregation of nanoclusters, which precipitate on the surface of SWy-2. Ca-rich U₆₀ aggregates associated with SWy-2 were identified and characterized by scanning electron microscopy with energy dispersive spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. This research enhances our understanding of the molecular-scale processes controlling U₆₀ behavior at the mineral–water interface.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); Univ. of Notre Dame, Notre Dame, IN (United States)

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

Grant/Contract Number:: SC0001089

OSTI ID:: 1566497

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 9 Vol. 53; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited By (1)

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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