Transformation of Ferrihydrite to Goethite and the Fate of Plutonium

Balboni, Enrica; Smith, Kurt F.; Moreau, Liane M.; Li, Tian T.; Maloubier, Melody; Booth, Corwin H.; Kersting, Annie B.; Zavarin, Mavrik

doi:10.1021/acsearthspacechem.0c00195

Transformation of Ferrihydrite to Goethite and the Fate of Plutonium

Journal Article · Tue Oct 27 00:00:00 EDT 2020 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.0c00195· OSTI ID:1811748

^[1]; Smith, Kurt F. ^[2]; Moreau, Liane M. ^[2]; Li, Tian T. ^[3]; Maloubier, Melody ^[4]; Booth, Corwin H. ^[2]; Kersting, Annie B. ^[1]; ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Clemson Univ., SC (United States); Laboratoire de Physique des 2 Infinis Irène Joliot Curie (IJCLab), Orsay (France)

Understanding the interactions between plutonium and iron (oxy)hydroxide minerals is necessary to gain a predictive understanding of plutonium environmental mobility and to evaluate long-term performance of nuclear waste repositories. We investigated the fate of plutonium during the formation of ferrihydrite and its subsequent transformation into goethite. Ferrihydrite was synthesized with varying quantities of Pu(IV) following either a sorption or coprecipitation process; the ferrihydrite was then aged hydrothermally to yield goethite. Additionally, the synthesized materials were characterized via extended X-ray absorption fine structure spectroscopy, transmission electron microscopy, and acid leaching to elucidate the nature of plutonium association with ferrihydrite and goethite. In samples prepared following the sorption method, plutonium was identified in two different forms: a PuO₂ precipitate and a surface-sorbed plutonium complex. For the samples prepared via coprecipitation, no PuO₂ formation occurs in the ferrihydrite precursor and in the goethite experiments where plutonium concentration is ≤1000 ppm (mg kg^–1). In these coprecipitation products, plutonium is strongly bound to the minerals either via formation of an inner sphere complex, or via an incorporation process. In the coprecipitation experiments, PuO₂ formation only occurs at the highest plutonium concentration (3000 ppm), suggesting that during ferrihydrite transformation into goethite, part of the plutonium can be remobilized to form PuO₂ nanoparticles. Collectively, our results demonstrate that the nature of plutonium associated with the precursor ferrihydrite (adsorbed vs coprecipitated) will have a direct impact on the association of plutonium with its alteration product (goethite). Furthermore, the data illustrate that some properties of plutonium association with the precursor ferrihydrite are retained through the transformation into goethite. These findings show that plutonium strongly associates with iron (oxy)hydroxides formed through coprecipitation processes and in these materials, plutonium can be strongly retained by the iron minerals.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

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

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1811748

Report Number(s):: LLNL-JRNL--812443; 1014445

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 11 Vol. 4; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Transformation of Ferrihydrite to Goethite and the Fate of Plutonium

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