Hydrothermal interactions of basalts with Cs and Sr of spent fuel elements. Implications to basalt as a nuclear waste repository

Sridhar Komarneni, Barry E. Scheetz

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10 Scopus citations

Abstract

The immobilization reactions of Cs, Sr, U and Mo from spent fuel elements (SFE) in the presence of basalts and basalt phases were investigated under hydrothermal, closed-system conditions. The exact Cs and Sr phases in SFE are not known with certainty, but Cs2MoO4, CsI, Cs2O, β-Cs2U2O7 and SrZrO3 are some of the predicted possibilities. These phases were mixed with basalts and basalt phases along with water, sealed in gold capsules and reacted at 100, 200 and 300°C under a confining pressure of 300 bars. The Cs and Sr concentrations of the product solutions were measured to determine the partitioning of these elements between the liquid and solid phases. Results varied substantially, depending on the particular basalt or basalt phase or Cs phase, the temperature and the duration of run. For example, a Deep Drill Hole (DDH-3) basalt-Cs2MoO4 reactions resulted in 15, 78 and 99% fixation of added Cs at 100, 200 and 300°C respectively. Fixation of up to 99.7 and 99.8% of the added Cs and Sr respectively were observed in some cases. X-Ray diffraction (XRD) analysis of the solid products revealed that Cs was immobilized by the formation of pollucite, (Cs, Na)AlSi2O6 in most cases and the formation of CsAlSiO4 in some cases. The interactions of basalts and basalt phases with Cs2MoO4 also resulted in the immobilization of Mo by the formation of powellite, CaMoO4 because Ca is available in the reaction mixtures. The U6+ in β-Cs2U2O7 was reduced to form uraninite, UO2 by the divalent iron component of basalts. The exact nature of Sr reaction with basalts is not clear because no new Sr phases could be detected by XRD. The reaction products, pollucite, CsAlSiO4, powellite and uraninite from SFE-basalt interactions serve to immobilize Cs, Mo and U because Cs in pollucite and CsAlSiO4 is difficult to exchange and Mo and U in powellite and uraninite are quite insoluble.

Original languageEnglish (US)
Pages (from-to)1967-1975
Number of pages9
JournalJournal of Inorganic and Nuclear Chemistry
Volume43
Issue number9
DOIs
StatePublished - 1981

All Science Journal Classification (ASJC) codes

  • Medicine(all)

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