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Trivalent Actinide Uptake by Iron (Hydr)oxides.

Nicolas Finck1, Sorin Nedel2, Knud Dideriksen2

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Am(III) retention on magnetite depends on formation pathway. Coprecipitation leads to Am incorporation into magnetite structure, while adsorption forms surface complexes with iron. Green rust precursor influences Am

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Area of Science:

  • Geochemistry
  • Radiochemistry
  • Materials Science

Background:

  • Understanding the fate of actinides like Americium(III) (Am(III)) in geological repositories is crucial for nuclear waste management.
  • Magnetite (Fe3O4) is a common mineral in geological environments and can influence radionuclide behavior.

Purpose of the Study:

  • To investigate the retention mechanisms of Am(III) by magnetite through coprecipitation and adsorption.
  • To elucidate the structural environment of Am(III) sorbed onto magnetite and its evolution over time.
  • To compare Am(III) incorporation in magnetite formed via different pathways, including a green rust precursor.

Main Methods:

  • X-ray absorption spectroscopy (XAS) to determine the local atomic environment of Am(III).
  • X-ray diffraction (XRD) for structural characterization of magnetite.
  • Solution chemistry to monitor Am(III) concentrations and speciation.

Main Results:

  • XAS data indicate Am(III) incorporation into Fe structural sites in magnetite during coprecipitation, forming Am-O-Fe bonds.
  • Aging of Am(III)-magnetite samples resulted in structural reorganization and increased order around Am.
  • Am(III) formed surface complexes with cosorbed Fe on preformed magnetite, influenced by Fe concentration.
  • In a green rust pathway, Am(III) occupied different sites in the precursor and intermediate phases before magnetite formation.

Conclusions:

  • The pathway of magnetite formation significantly impacts the extent and location of Am(III) incorporation.
  • Coprecipitation allows for deeper structural integration of Am(III) within magnetite compared to surface complexation.
  • The mineral precursor and reaction conditions dictate the actinide's final structural environment.