GSA 2020 Connects Online

Paper No. 148-19
Presentation Time: 4:45 PM

CAPTURE OF URANYL PEROXIDE NANOCLUSTERS INTO PILLARED HYDROTALCITES


PERRY, Samuel N., Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, 301 Stinson-Remick Hall, Notre Dame, IN 46556, MILLS, Stuart J., Geosciences, Museums Victoria, Melbourne, GPO Box 666, Melbourne, VIC 3001, Australia and BURNS, Peter C., Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, 301 Stinson-Remick Hall, Notre Dame, IN 46556; Chemistry and Biochemistry, University of Notre Dame, 301 Stinson-Remick Hall, Notre Dame, IN 46556

U contamination in the subsurface is a persistent issue at sites around the world, such as locations involved in the Manhattan Project or defunct mining districts. U poses a significant health hazard to humans, with the US EPA having imposed a 30 ppb limit in drinking water. In the presence of H2O2 in alkaline aqueous solutions, U self assembles into large, hollow polyoxometalates (POMs) referred to as uranyl peroxide nanoclusters [1]. These macroions can be relatively large, with diameters over 3 nm, and their surface topologies can be modified through the incorporation of oxyanions such as oxalate or pyrophosphate [1]. These POMs are of interest for green nuclear energy production due to their potential applications in nuclear fuel reprocessing [2].

Layered double hydroxides (LDHs) are a class of layered compounds that have generated considerable interest in the past few decades and have been researched extensively for use in remediating toxic elements and organic compounds [3]. Their applications can be enhanced through expansion of the interlayer to heights of ~4 nm [4], allowing for potential capture of large POMs.

Mg-Al LDHs were coprecipitated with an organic anion acting as a pillar, characterized with PXRD, TGA and ICP-OES, then reacted with aqueous solutions of uranyl peroxide nanoclusters. The greatest removal of U was observed when the initial POM solutions contained pyrophosphate-bearing uranyl peroxide nanoclusters. The batch reactions suggest LDH interactions with uranyl peroxide nanoclusters can be controlled, allowing for storage of U in an intermediate form or released back into solution as a nanocluster. As a non-toxic phase that is easily manufactured, pillared MgAl-LDHs show potential for applications in environmental remediation of U.

[1] Burns, et al. Angew. Chem. Int. Ed. 44 (2005) 2135-2139.

[2] Wylie, et al. J. Nucl. Mater. 473 (2016) 125-130.

[3] Li & Duan. Struct. Bond. 119 (2006) 193-223.

[4] Clearfield, et al. J. Incl. Phenom. Mol. Recognit. Chem. 11 (1991) 361-378.