Dissolution of poorly soluble uranyl phosphate phases in the Metaautunite Subgroup under uranyl peroxide cage cluster forming conditions

Lobeck, Haylie L.; Balboni, Enrica; Parker, Connor J.; Kohlgruber, Tsuyoshi A.; Xu, Mengyu; Boukdad, Sara; Ridder, Henry M.; Traustason, Hrafn; Isner, Jordan K.; Dzik, Ewa A.; Burns, Peter C.

doi:10.2138/am-2020-7106

Title: Dissolution of poorly soluble uranyl phosphate phases in the Metaautunite Subgroup under uranyl peroxide cage cluster forming conditions

Journal Article · Thu Jan 23 00:00:00 EST 2020 · American Mineralogist

DOI:https://doi.org/10.2138/am-2020-7106· OSTI ID:1811761

Lobeck, Haylie L. ^[1]; Balboni, Enrica ^[2]; Parker, Connor J. ^[3]; Kohlgruber, Tsuyoshi A. ^[1]; Xu, Mengyu ^[1]; Boukdad, Sara ^[1]; Ridder, Henry M. ^[1]; Traustason, Hrafn ^[1]; Isner, Jordan K. ^[1]; Dzik, Ewa A. ^[1];

^[1]

Univ. of Notre Dame, IN (United States)
Univ. of Notre Dame, IN (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of Notre Dame, IN (United States); Clemson Univ., SC (United States)

Uranyl phosphate minerals are widespread in uranium deposits and usually exhibit very low solubility in aqueous systems. Uranyl phosphates of the autunite group and metaautunite subgroup impact the mobility of uranium in the environment and have inspired groundwater remediation strategies that emphasize their low solubility. The importance of soluble uranium-bearing macro-anions, including nanoscale uranyl peroxide cage clusters, is largely unexplored relative to solubilization of normally low-solubility uranium minerals. Eight synthetic analogs of metaautunite subgroup minerals have been prepared and placed in various alkaline aqueous solutions containing hydrogen peroxide and tetraethylammonium hydroxide. Each uranyl phosphate studied has a topologically identical anionic sheet of uranyl square bipyramids and phosphate tetrahedra combined with various cations (Li⁺, Na⁺, K⁺, Rb⁺, Cs⁺, Mg²⁺, Ca²⁺, Ba²⁺) and water in the interlayer. Uranyl peroxides formed under many of the experimental conditions examined, including solid studtite [(UO₂)(O₂)(H₂O)₂](H₂O)₂ and soluble uranyl peroxide cage clusters containing as many as 28 uranyl ions. Uranyl phosphate solids in contact with solutions in which uranyl peroxide cage clusters formed dissolved extensively or completely. The greatest dissolution of uranyl phosphates occurred in systems that contained cations with larger hydrated radii, Li⁺ and Na⁺. The details of the uranium speciation in solution depended on the pH and counter cations provided from the interlayers of the uranyl phosphate solids.

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Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of Notre Dame, IN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344; NA0003763

OSTI ID:: 1811761

Alternate ID(s):: OSTI ID: 1596357

Report Number(s):: LLNL-JRNL-786890; 965811; TRN: US2213197

Journal Information:: American Mineralogist, Vol. 105, Issue 2; ISSN 0003-004X

Publisher:: Mineralogical Society of AmericaCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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metaautunite
dissolution
uranium
studtite
uranyl peroxide nanoclusters
peroxide
uranyl phosphate

Title: Dissolution of poorly soluble uranyl phosphate phases in the Metaautunite Subgroup under uranyl peroxide cage cluster forming conditions

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