Micro-focused synchrotron radiation techniques to investigate actinide elements in geological samples are becoming an increasingly used tool in nuclear waste disposal research. In this article, results using mu-focus techniques are presented from a bore core section of a U-rich tertiary sediment collected from Ruprechtov, Czech Republic, a natural analog to nuclear waste repository scenarios in deep geological formations. Different methods are applied to obtain various, complementary information. Elemental and element chemical state distributions are obtained from micro-XRF measurements, oxidation states of As determined from micro-XANES, and the crystalline structure of selected regions are studied by means of micro-XRD. We find that preparation of the thin section created an As oxidation state artifact; it apparently changed the As valence in some regions of the sample. Results support our previously proposed hypothesis of the mechanism for U-enrichment in the sediment. AsFeS coating on framboid Fe nodules in the sediment reduced mobile groundwater-dissolved U(VI) to less-soluble U(IV), thereby immobilizing the uranium in the sediment.
Investigations by micrometer-scale X-ray fluorescence and X-ray absorption fine structure (micro-XRF and micro-XAFS) recorded in a confocal geometry on a bore core section of a uranium-rich tertiary sediment are performed in order to assess mechanisms leading to immobilization of the uranium during diagenesis. Results show uranium to be present as a tetravalent phosphate and that U(IV) is associated with As(V). Arsenic present is either As(V) or As(O); we found no evidence for As(III). The As(O) is observed to be intimately associated with the surface of Fe(II) nodules and likely arsenopyrite. A hypothesis for the mechanism of uranium immobilization is proposed, where arsenopyrite acted as reductant of groundwater-dissolved U(VI), leading to precipitation of less soluble U(IV) and thereby forming As(V).
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