Identification of simultaneous U(VI) sorption complexes and U(IV) nanoprecipitates on the magnetite (111) surface

Singer, David M; Chatman, Shawn ME; Ilton, Eugene S; Rosso, Kevin M; Banfield, Jillian F; Waychunas, Glenn

doi:10.1021/es203877x

Title: Identification of simultaneous U(VI) sorption complexes and U(IV) nanoprecipitates on the magnetite (111) surface

Journal Article · Tue Apr 03 00:00:00 EDT 2012 · Environmental Science & Technology, 46(7):3811-3820

DOI:https://doi.org/10.1021/es203877x· OSTI ID:1040672

Singer, David M; Chatman, Shawn ME; Ilton, Eugene S; Rosso, Kevin M; Banfield, Jillian F; Waychunas, Glenn

Sequestration of uranium (U) by magnetite is a potentially important sink for U in natural and contaminated environments. However, molecular-scale controls which favor U(VI) uptake including both adsorption of U(VI) and reduction to U(VI) by magnetite remain poorly understood, in particular the role of U(VI)-CO3-Ca complexes in inhibiting U(VI) reduction. To investigate U uptake pathways on magnetite as a function of U(VI) aqueous speciation, we performed batch sorption experiments on (111) surfaces of natural single crystals under a range of solution conditions (pH 5 and 10; 0.1 mM U(VI); 1 mM NaCl; and with or without 0.5 mM CO3 and 0.1 mM Ca) and characterized surface-associated U using grazing incidence extended x-ray absorption fine structure spectroscopy (GI-EXAFS), grazing incidence x-ray diffraction (GI-XRD), and scanning electron microscopy (SEM). In the absence of both carbonate ([CO3]T, denoted here as CO3) and calcium (Ca), or in the presence of CO3 only, co-existing adsorption of U(VI) surface species and reduction to U(IV) occurs at both pH 5 and 10. In the presence of both CO3 and Ca, only adsorption of U(VI) occur. When U reduction occurs, nanoparticulate UO2 forms only within and adjacent to surface microtopographic features such as crystal boundaries and cracks. This result suggests that U reduction is limited to defect-rich surface regions. Further, at both pH 5 and 10 in the presence of both CO3 and Ca, U(VI)-CO3-Ca ternary surface species develop and U reduction is precluded. These findings extend the range of conditions under which U (VI)-CO3-Ca complexes inhibit U reduction.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1040672

Report Number(s):: PNNL-SA-83908; 39953; 42318; KP1702030

Journal Information:: Environmental Science & Technology, 46(7):3811-3820, Journal Name: Environmental Science & Technology, 46(7):3811-3820

Country of Publication:: United States

Language:: English

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